能源化学(英文)
ISSN 1003-9953
     
能源化学(英文)

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Tang, Titirici, and Zhang reviewed the roles of nanocarbons and material design principles for energy electrocatalysis. The multifunctionalities of nanocarbon substrates (accelerating the electron and mass transport, regulating the incorporation of active components, manipulating electron structures, generating confinement effects, assembly into 3D free-standing electrodes) and the intrinsic activity of nanocarbon catalysts (multi-heteroatom doping, hierarchical structure, topological defects) are discussed systematically. This review is inspiring for more insights and methodical research in mechanism understanding, material design, and device optimization of energy electrocatalysis.


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2017, Vol.26 No.6   刊出日期: 2017-11-15
本期栏目: Preface | Reviews | Articles |
 
 
Preface
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Preface to Special Issue: Advanced Energy Chemistry for Electrocatalysis
Qiang Zhang, Jintao Zhang, Yu Chen
2017 Vol. 26 (6): 0-0 [摘要] ( 118 ) [HTML 1KB] [PDF] ( 0 )

When the cost of renewable energy harvest from solar and wind is competitive with the prices of electricity from irreversible resources like coals, the electricity would be one of the most powerful and sustainable driving force for the future chemical reactions. Therefore, much effort has been devoted into the development of advanced energy chemistry on the basis of the motivated electrocatalysis.
Among various electrocatalysis reactions, the hydrogen and oxygen related electrocatalysis processes are strongly considered [1]. For instance, the oxygen reduction reaction (ORR) is the core step and bottleneck of many sustainable energy-conversion technologies toward an efficient, smart, and green future [2,3]. Specifically, ORR is the dominant reaction on the cathodes of fuel cells and metal–air batteries [4]. The oxygen evolution reaction (OER) constitutes the bottleneck in water splitting [5]. Additionally, OER is also coupled with various renewable energy systems such as solar cells, metal-air batteries, and fuel cells. The multi-electron reaction process for ORR/OER suffers from sluggish kinetics and high overpotential, which requires high-performance electrocatalysts for practical applications and has stimulated intense research interest. For instance, on the 2nd China International Symposium on Energy Materials and Chemistry held in Changsha, 2017.6.9-12, a special session of electrocatalysis was proposed and attracted many attendees working on energy chemistry. The innovation on the energy chemistry of electrocatalysis introduces not only emerging principles on a family of advanced electrocatalyst (such as precious metal, metal oxide/nitride/carbide, metal-free catalyst, and carbon based electrocatalyst) [6–8], but also of many potential electrocatalysis processes (e.g. precious metal-free ORR, OER, hydrogen evolution reaction, hydrogen oxidation reaction, carbon dioxide reduction reaction, chlorine evolution reaction, nitrogen reduction reaction).
Along with the rapid development of scientific researches and industrial applications on the science and technology of energy chemistry for electrocatalysis, a special issue on Journal of Energy Chemistry titled “Advanced Energy Chemistry for Electrocatalysis” is now dedicated to the interested readers. This special issue contains 7 review articles and 17 research papers. The topics cover different areas of energy chemistry for electrocatalysis, including electrocatalyst preparation, catalytic mechanism discussion, and the specific applications. Typically, catalytic conversion of CO2 is a promising solution to address global warming and energy shortage issues. Wu, Li, and co-workers [9] review the reaction mechanisms and possible pathways for productions of solar fuels from CO2 on Cu-based catalysts. Zhang and coworkers [10] demonstrate the fundamental principles for enhancing the electrocatalytic activity and selectivity of Cu-based electrocatalyst for CO2 reduction reaction (CRR), highlighting the novel insights into the rational design of advanced electrocatalysts for CRR. Direct methanol fuel cells is the most attractive energy technology for sustainable society, however, its practical applications are heavily hindered by the sluggish methanol oxidation reaction (MOR) and ORR electrocatalysts. Xia, Chen, and coworkers [11] summarize recent advances of unsupported Pt-based electrocatgalysts and highlight the relationship between the MOR performance and structure tailoring and composition modulating strategies. Zhang and coworkers [12] afford an in-depth digestion of present achievements on the role of nanocarbons and material design principles for ORR. The intrinsic activity of nanocarbon electrocatalysts and their multifunctional applications are presented systematically with perspectives on the further research in this rising research field. As an emerging kind of electrocatalyst, layered double hydroxides and their derivatives reviewed by Shao and co-workers [13] have been adopted as efficient electrocatalysts and exhibited superb activity and remarkable durability in ORR, OER, HER, and CRR. Additionally, NH3 is a vital emerging energy carrier and storage medium in the future hydrogen economy. Thus, the nitrogen reduction reaction (NRR) is another emerging direction in the field of electrocatalysis. The electrochemical NRR routes exhibit the promising potential to reduce the energy consumption. Ma and coworkers [14] present the recent advances in ammonia synthesis electrocatalyzed by a series of functional materials in this special issue. To rational design of advanced electrocatalysts for vast electrocatalysis process, Zhang and coworkers [15] present useful information about the microstructures and chemical compositions of the electrocatalysts on nano and atomic scale by using transmission electron microscopy, which is of importance for establishing the synthesis-structure-performance relationship. The recent research progress in the field of energy-related electrocatalysis on the basis of experimental observation and theoretical simulation from the leading scientists are also included in this special issue.
This special issue represents a distinguished effort of the authors and anonymous referees, editors who really make the issue fruitful. We would like to thank them for the generous contribution. We also invite our readers to get more information on our website of Journal of Energy Chemistry (http://www.sciencedirect.com/journal/journal-of-energy-chemistry), which involves the creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies.

Reviews
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Recent advances in Cu-based nanocomposite photocatalysts for CO2 conversion to solar fuels
Huan Xie, Jingyun Wang, Kemakorn Ithisuphalap, Gang Wu, Qing Li
2017 Vol. 26 (6): 1039-1049 [摘要] ( 172 ) [HTML 1KB] [PDF] ( 0 )

CO2 conversion via photocatalysis is a potential solution to address global warming and energy shortage. Photocatalysis can directly utilize the inexhaustible sunlight as an energy source to catalyze the reduction of CO2 to useful solar fuels such as CO, CH4, CH3OH, and C2H5OH. Among studied formulations, Cubased photocatalysts are the most attractive for CO2 conversion because the Cu-based photocatalysts are low-cost and abundance comparing noble metal-based catalysts. In this literature review, a comprehensive summary of recent progress on Cu-based photocatalysts for CO2 conversion, which includes metallic copper, copper alloy nanoparticles (NPs), copper oxides, and copper sulfides photocatalysts, can be found. This review also included a detailed discussion on the correlations of morphology, structure, and performance for each type of Cu-based catalysts. The reaction mechanisms and possible pathways for productions of various solar fuels were analyzed, which provide insight into the nature of potential active sites for the catalysts. Finally, the current challenges and perspective future research directions were outlined, holding promise to advance Cu-based photocatalysts for CO2 conversion with much-enhanced energy conversion efficiency and production rates.

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Rational design of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide
Baohua Zhang, Jintao Zhang
2017 Vol. 26 (6): 1050-1066 [摘要] ( 148 ) [HTML 1KB] [PDF] ( 0 )

The recent development of Cu-based electrocatalysts for electrochemical reduction of carbon dioxide (CO2) has attracted much attention due to their unique activity and selectivity compared to other metal catalysts. Particularly, Cu is the unique electrocatalyst for CO2 electrochemical reduction with high selectivity to generate a variety of hydrocarbons. In this review, we mainly summarize the recent advances on the rational design of Cu nanostructures, the composition regulation of Cu-based alloys, and the exploitation of advanced supports for improving the catalytic activity and selectivity toward electrochemical reduction of CO2. The special focus is to demonstrate how to enhance the activity and selectivity of Cubased electrocatalyst for CO2 reduction. The perspectives and challenges for the development of Cu-based electrocatalysts are also addressed. We hope this review can provide timely and valuable insights into the design of advanced electrocatalytic materials for CO2 electrochemical reduction.

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Research advances in unsupported Pt-based catalysts for electrochemical methanol oxidation
Xin Long Tian, Lijuan Wang, Peilin Deng, Yu Chen, Bao Yu Xia
2017 Vol. 26 (6): 1067-1076 [摘要] ( 117 ) [HTML 1KB] [PDF] ( 0 )

Direct methanol fuel cells are one of the most promising alternative energy technologies in the foreseeable future, but its successful commercialization in large scale is still heavily hindered by several technical shortfalls, especially the undesirable activity and durability issues of electrocatalysts toward methanol oxidation reaction. In light of these challenges, the inherent advantages of unsupported Pt based nanostructures demonstrate their great potentials as durable and efficient electrocatalysts for direct methanol fuel cells. This review will summarize recent achievements of unsupported Pt-based electrocatalysts toward methanol oxidation, with highlighting the interactions between the performance and structure tailoring and composition modulating. At last, a perspective is proposed for the upcoming challenges and possible opportunities to further prompt the practical application of unsupported Pt-based electrocatalysts for direct methanol fuel cells.

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A review of nanocarbons in energy electrocatalysis:Multifunctional substrates and highly active sites
Cheng Tang, Maria-Magdalena Titirici, Qiang Zhang
2017 Vol. 26 (6): 1077-1093 [摘要] ( 126 ) [HTML 1KB] [PDF] ( 0 )

Nanocarbons are of progressively increasing importance in energy electrocatalysis, including oxygen reduction, oxygen evolution, hydrogen evolution, CO2 reduction, etc. Precious-metal-free or metal-free nanocarbon-based electrocatalysts have been revealed to potentially have effective activity and remarkable durability, which is promising to replace precious metals in some important energy technologies, such as fuel cells, metal-air batteries, and water splitting. In this review, rather than overviewing recent progress completely, we aim to give an in-depth digestion of present achievements, focusing on the different roles of nanocarbons and material design principles. The multifunctionalities of nanocarbon substrates (accelerating the electron and mass transport, regulating the incorporation of active components, manipulating electron structures, generating confinement effects, assembly into 3D free-standing electrodes) and the intrinsic activity of nanocarbon catalysts (multi-heteroatom doping, hierarchical structure, topological defects) are discussed systematically, with perspectives on the further research in this rising research field. This review is inspiring for more insights and methodical research in mechanism understanding, material design, and device optimization, leading to a targeted and high-efficiency development of energy electrocatalysis.

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Advances in efficient electrocatalysts based on layered double hydroxides and their derivatives
Lei Zhou, Mingfei Shao, Min Wei, Xue Duan
2017 Vol. 26 (6): 1094-1106 [摘要] ( 115 ) [HTML 1KB] [PDF] ( 0 )

The explore and development of electrocatalysts have gained significant attention due to their indispensable status in energy storage and conversion systems, such as fuel cells, metal-air batteries and solar water splitting cells. Layered double hydroxides (LDHs) and their derivatives (e.g., transition metal alloys, oxides, sulfides, nitrides and phosphides) have been adopted as catalysts for various electrochemical reactions, such as oxygen reduction, oxygen evolution, hydrogen evolution, and CO2 reduction, which show excellent activity and remarkable durability in electrocatalytic process. In this review, the synthesis strategies, structural characters and electrochemical performances for the LDHs and their derivatives are described. In addition, we also discussed the effect of electronic and geometry structures to their electrocatalytic activity. The further development of high-performance electrocatalysts based on LDHs and their derivatives is covered by both a short summary and future outlook from the viewpoint of the material design and practical application.

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Lowering reaction temperature:Electrochemical ammonia synthesis by coupling various electrolytes and catalysts
Xinghua Guo, Yunpei Zhu, Tianyi Ma
2017 Vol. 26 (6): 1107-1116 [摘要] ( 105 ) [HTML 1KB] [PDF] ( 0 )

Ammonia is a vital emerging energy carrier and storage medium in the future hydrogen economy, even presenting relevant advantages compared with methanol due to the higher hydrogen content (17.6 wt% for ammonia versus 12.5 wt% for methanol). The rapidly growing demand for ammonia is still dependent on the conventional high-temperature and high-pressure Haber-Bosch process, which can deliver a conversion rate of about 10%-15%. However, the overall process requires a large amount of fossil fuels, resulting in serious environmental problems. Alternatively, electrochemical routes show the potential to greatly reduce the energy consumption, including sustainable energy sources and simplify the reactor design. Electrolytes perform as indispensable reaction medium during electrochemical processes, which can be further classified into solid oxide electrolytes, molten salt electrolytes, polymer electrolytes, and liquid electrolytes. In this review, recent developments and advances of the electrocatalytic ammonia synthesis catalyzed by a series of functional materials on the basis of aforementioned electrolytes have been summarized and discussed, along with the presentation and evaluation of catalyst preparation, reaction parameters and equipment.

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A review of electrocatalyst characterization by transmission electron microscopy
Liyun Zhang, Wen Shi, Bingsen Zhang
2017 Vol. 26 (6): 1117-1135 [摘要] ( 116 ) [HTML 1KB] [PDF] ( 0 )

At present, the development of highly efficient electrocatalysts with more rational control of microstructures (e.g. particle size, morphology, surface structure, and electronic structure) and chemical composition is needed and remained great challenges. Transmission electron microscopy (TEM) can offer the information about the microstructures and chemical compositions of the electrocatalysts on nano and atomic scale, which enables us to establish the synthesis-structure-performance relationship and further direct the design of new electrocatalysts with high performance. In this minireview paper, a brief introduction on the basic characterization of electrocatalysts with TEM, followed by the studying of dynamic evolution of the electrocatalysts in electrochemical reactions with identical location-TEM, is discussed.

Articles
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The Co3O4 nanosheet array as support for MoS2 as highly efficient electrocatalysts for hydrogen evolution reaction
Xiao Sun, Jia Huo, Yide Yang, Lei Xu, Shuangyin Wang
2017 Vol. 26 (6): 1136-1139 [摘要] ( 110 ) [HTML 1KB] [PDF] ( 0 )

The electrochemical hydrogen evolution reaction (HER) on a non-precious electrocatalyst in an alkaline environment is of essential importance for future renewable energy. The design of advanced electrocatalysts for HER is the most important part to reduce the cost and to enhance the efficiency of water splitting. MoS2 is considered as one of the most promising electrocatalysts to replace the precious Pt catalyst. Herein, for the first time, we have successfully loaded MoS2 electrocatalysts onto the Co3O4 nanosheet array to catalyze HER with a low onset potential of ~76 mV. The high hydrogen evolution activity of MoS2 supported on the Co3O4 nanosheet array may be attributed to the increased active sites and the electronic interactions between MoS2 and Co3O4.

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In-situ carbonization approach for the binder-free Ir-dispersed ordered mesoporous carbon hydrogen evolution electrode
Yanghua He, Jinming Xu, Fanan Wang, Xiaochen Zhao, Guangzhao Yin, Qing Mao, Yanqiang Huang, Tao Zhang
2017 Vol. 26 (6): 1140-1146 [摘要] ( 96 ) [HTML 1KB] [PDF] ( 0 )

A binder-free Ir-dispersed ordered mesoporous carbon (Ir-OMC) catalytic electrode has been prepared through a designed in-situ carbonization method, which involves coating resorcinol and formaldehyde mixtures with iridium precursors onto the three-dimensional nickel foam framework, followed by insitu calcination in N2 atmosphere at 800℃ for 3 h. This electrode shows a large surface area, ordered mesoporous structure and homogeneous distribution of metal nanoparticles. It presents good activity and stability towards hydrogen evolution reaction, which is attributed to the efficient mass and electron transport from the intimate contact among Ir nanoparticles, ordered mesoporous carbon matrix and 3D conductive substrate. We hope that this in-situ carbonization synthetic route can also be applied to design more high-performance catalysts for water splitting, fuel cells and other clean energy devices.

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Glucose-derived carbon sphere supported CoP as efficient and stable electrocatalysts for hydrogen evolution reaction
Bangde Luo, Ting Huang, Ye Zhu, Deli Wang
2017 Vol. 26 (6): 1147-1152 [摘要] ( 118 ) [HTML 1KB] [PDF] ( 0 )

Glucose-derived carbon sphere supported cobalt phosphide nanoparticles (CoP/C) were synthesized via a concise two-step method. The electrochemical measurement results indicate that the CoP/C prepared at 900℃ presents excellent electrocatalytic performance for hydrogen evolution reaction (HER). The overpotential at a current density of 10 mA cm-2 is 108 and 163 mV in 0.5 M H2SO4 and 1 M KOH, respectively, and maintains its electrocatalytic durability for at least 10 h. This work supplies a new field to challenge the construction of electrocatalysts for HER through using cost-effective carbon supported transition metal phosphides.

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Polyethyleneimine modified AuPd@PdAu alloy nanocrystals as advanced electrocatalysts towards the oxygen reduction reaction
Qi Xue, Guangrui Xu, Rundong Mao, Huimin Liu, Jinghui Zeng, Jiaxing Jiang, Yu Chen
2017 Vol. 26 (6): 1153-1159 [摘要] ( 111 ) [HTML 1KB] [PDF] ( 0 )

Designing the low cost, active, durable, and alcohol-tolerant cathode catalysts towards the oxygen reduction reaction (ORR) is significant for the large-scale commercialization of direct alcohol fuel cells. Recently, Pd-based nanocrystals have attracted attention as Pt-alternative cathode catalysts towards the ORR in the alkaline electrolyte. Unfortunately, the pristine Pd-based nanocrystals lack the selectivity towards the ORR due to their inherent activity for the alcohol molecule oxidation reaction in the alkaline electrolyte. In this work, polyethyleneimine (PEI) modified AuPd alloy nanocrystals with Au-rich AuPd alloy cores and Pd-rich PdAu alloy shells (AuPd@PdAu-PEI) are successfully synthesized using a traditional chemical reduction method in presence of PEI. The rotating disk electrode (RDE) technique is applied to evaluate the ORR performance of AuPd@PdAu-PEI nanocrystals. Compared with commercial Pd black, AuPd@PdAu-PEI nanocrystals show significantly enhanced activity and durability towards the ORR, and simultaneously exhibit particular alcohol tolerance towards the ORR in the alkaline electrolyte.

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In situ constructing of ultrastable ceramic@graphene core-shell architectures as advanced metal catalyst supports toward oxygen reduction
Hui Wu, Tao Peng, Zongkui Kou, Kun Cheng, Jie Zhang, Jian Zhang, Tian Meng, Shichun Mu
2017 Vol. 26 (6): 1160-1167 [摘要] ( 121 ) [HTML 1KB] [PDF] ( 0 )

The changeable structure of 2D graphene nanosheets makes the Pt-based nanoparticles (NPs) possess a low efficiency toward oxygen reduction reaction (ORR) and a short lifetime for proton exchange membrane fuel cells. Thus, a unique TiC@graphene core-shell structure material with low surface energy is designed and prepared by an in situ forming strategy, and firstly applied as a stable support of Pt NPs. The as-prepared Pt/GNS@TiC catalyst presents a high activity. Especially, its ORR stability is remarkably improved. Even after 15000 potential cycles, the half-wave potential and mass activity toward ORR have almost no change. This can be attributed to that the graphene nanosheet existing in a sphere shape effectively avoids the restacking or folding caused by the giant surface tension in 2D graphene nanosheets, impeding the decrease of the triple-phase boundary on Pt NPs. Significantly, the power density of fuel cells with our novel catalyst reaches 853 mV cm-2 under a low Pt loading (0.25 mgPt cm-2) and H2/Air conditions. These indicate the new ceramic@graphene core-shell nanocomposite is a promising application in fuel cells and other fields.

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Highly efficient iron-nitrogen electrocatalyst derived from covalent organic polymer for oxygen reduction
Jianing Guo, Mengyao Ning, Zhonghua Xiang
2017 Vol. 26 (6): 1168-1173 [摘要] ( 111 ) [HTML 1KB] [PDF] ( 0 )

Developing non-precious metal catalyst with high activity, good stability and low cost for electrocatalytic oxygen reduction reaction (ORR) is critical for the wide application of energy conversion system. Here, we developed a cost-effective synthetic strategy via silica assistance to obtain a novel Fe3C/Fe-Nx-C (named as COPBP-PB-Fe-900-SiO2) catalyst with effective active sites of Fe-Nx and Fe3C from the rational design two-dimensional covalent organic polymer (COPBP-PB). The nitrogen-rich COP effectively promotes the formation of active Fe-Nx sites. Additionally, the silica not only can effectively suppress the formation of large Fe-based particles in the catalysts, but also increases the degree of carbonization of the catalyst. The as-prepared COPBP-PB-Fe-900-SiO2 catalyst exhibits high electrocatalytic activity for ORR with a halfwave potential of 0.85 V vs. reversible hydrogen electrode (RHE), showing comparable activity as compared with the commercial Pt/C catalysts in alkaline media. Moreover, this catalyst also shows a high stability with a nearly constant onset potential and half-wave potential after 10,000 cycles. The present work is highly meaningful for developing ORR electrocatalysts toward wide applications.

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Two-step pyrolysis of ZIF-8 functionalized with ammonium ferric citrate for efficient oxygen reduction reaction
Yifan Ye, Fan Cai, Chengcheng Yan, Yanshuo Li, Guoxiong Wang, Xinhe Bao
2017 Vol. 26 (6): 1174-1180 [摘要] ( 109 ) [HTML 1KB] [PDF] ( 0 )

Zeolitic imidazolate frameworks (ZIFs) are widely employed in catalyst synthesis as parental materials for electrochemical energy storage and conversion. Herein, we have demonstrated a facile synthesis of highly efficient catalyst for oxygen reduction reaction in both alkaline and acidic medium, which is derived from ZIF-8 functionalized with ammonium ferric citrate via two-step pyrolysis in Ar and NH3 atmosphere. The results reveal that the catalytic activity improvement after NH3 pyrolysis benefits from mesoporedominated morphology and high utilization of Fe-containing active sites. The optimum catalyst shows excellent performance in zinc-air battery and polymer electrolyte membrane fuel cell tests.

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Nitrogen-doped carbon nanotube encapsulating cobalt nanoparticles towards efficient oxygen reduction for zinc-air battery
Haihua Wu, Xiaole Jiang, Yifan Ye, Chengcheng Yan, Songhai Xie, Shu Miao, Guoxiong Wang, Xinhe Bao
2017 Vol. 26 (6): 1181-1186 [摘要] ( 113 ) [HTML 1KB] [PDF] ( 0 )

Nitrogen-doped carbon materials encapsulating 3d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction (ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube (N-CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N-CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc-air battery.

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Characterization of Fe/N-doped graphene as air-cathode catalyst in microbial fuel cells
Dingling Wang, Zhaokun Ma, Yang'en Xie, Huaihe Song
2017 Vol. 26 (6): 1187-1195 [摘要] ( 114 ) [HTML 1KB] [PDF] ( 0 )

This work proposed a simple and efficient approach for synthesis of durable and efficient non-precious metal oxygen reduction reaction (ORR) electro-catalysts in MFCs. The rod-like carbon nanotubes (CNTs) were formed on the Fe-N/SLG sheets after a carbonization process. The maximum power density of 1210 ±23 mW·m-2 obtained with Fe-N/SLG catalyst in an MFC was 10.7% higher than that of Pt/C catalyst (1080±20 mW·m-2) under the same condition. The results of RDE test show that the ORR electron transfer number of Fe-N/SLG was 3.91 ±0.02, which suggested that ORR catalysis proceeds through a four-electron pathway. The whole time of the synthesis of electro-catalysts is about 10 h, making the research take a solid step in the MFC expansion due to its low-cost, high efficiency and favorable electrochemical performance. Besides, we compared the electrochemical properties of catalysts using SLG, high conductivity graphene (HCG, a kind of multilayer graphene) and high activity graphene (HAG, a kind of GO) under the same conditions, providing a solution for optimal selection of cathode catalyst in MFCs. The morphology, crystalline structure, elemental composition and ORR activity of these three kinds of Fe-N/C catalysts were characterized. Their ORR activities were compared with commercial Pt/C catalyst. It demonstrates that this kind of Fe-N/SLG can be a type of promising highly efficient catalyst and could enhance ORR performance of MFCs.

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Integrated Ni2P nanosheet arrays on three-dimensional Ni foam for highly efficient water reduction and oxidation
Jintao Ren, Zhongpan Hu, Chong Chen, Yuping Liu, Zhongyong Yuan
2017 Vol. 26 (6): 1196-1202 [摘要] ( 114 ) [HTML 1KB] [PDF] ( 0 )

The large-scale synthesis of efficient nonprecious bifunctional electrocatalysts for overall water splitting is a great challenge for future renewable energy conversion systems. Herein, Ni2P nanosheet arrays directly grown on three-dimensional (3D) Ni foam (NiP/NF) are fabricated by hydrothermal treatment of metallic Ni foam with H2O2 solution and subsequent phosphidation with NaH2PO2. The NiP/NF as electrocatalyst exhibits superior activities for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Most importantly, employing both as the cathode and anode for an alkaline water electrolyzer, NiP/NF only requires a cell voltage of 1.63 V to reach a current density of 10 mV cm-2, together with stronger durability. Preliminary catalytic information suggests that the tailored 3D superstructure and integrated electrode configurations afford improved active sties and enhanced electron/mass transfer, responding for the outstanding activity and stability.

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Assembling Co9S8 nanoflakes on Co3O4 nanowires as advanced core/shell electrocatalysts for oxygen evolution reaction
Shengjue Deng, Shenghui Shen, Yu Zhong, Kaili Zhang, Jianbo Wu, Xiuli Wang, Xinhui Xia, Jiangping Tu
2017 Vol. 26 (6): 1203-1209 [摘要] ( 109 ) [HTML 1KB] [PDF] ( 0 )

Rational design of advanced cost-effective electrocatalysts is vital for the development of water electrolysis. Herein, we report a novel binder-free efficient Co9S8@Co3O4 core/shell electrocatalysts for oxygen evolution reaction (OER) via a combined hydrothermal-sulfurization method. The sulfurized net-like Co9S8 nanoflakes are strongly anchored on the Co3O4 nanowire core forming self-supported binder-free core/shell electrocatalysts. Positive advantages including larger active surface area of Co9S8 nanoflakes, and reinforced structural stability are achieved in the Co9S8@Co3O4 core/shell arrays. The OER performances of the Co9S8@Co3O4 core/shell arrays are thoroughly tested and enhanced electrocatalytic performance with lower over-potential (260 mV at 20 mA cm-2) and smaller Tafel slopes (56 mV dec-1) as well as long-term durability are demonstrated in alkaline medium. Our proposed core/shell smart design may provide a new way to construct other advanced binder-free electrocatalysts for applications in electrochemical catalysis.

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PVP-assisted synthesis of porous CoO prisms with enhanced electrocatalytic oxygen evolution properties
Xueli Zhao, Wei Zhang, Rui Cao
2017 Vol. 26 (6): 1210-1216 [摘要] ( 109 ) [HTML 1KB] [PDF] ( 0 )

Hollow metal oxide materials with nanometer-to-micrometer dimensions have attracted tremendous attention because of their potential applications in energy conversion and storage systems. Numerous efforts have been focused on developing versatile methods for the rational synthesis of various hollow structures to act as efficient water oxidation catalysts. In this work, a unique porous and hollow CoO tetragonal prism-like structure has been successfully synthesized via a facile and efficient co-precipitation method with polyvinylpyrrolidone (PVP K30) followed by a heating treatment of the resulted precipitates. The as-prepared porous and hollow CoO microprisms displayed a high activity and stability for water oxidation in 1.0 M KOH solution. To reach a current density of 10 mA/cm2, a low overpotential of 280 mV is required. The remarkable activity can be attributed to the synergistic effect between two different but well-distributed CoO crystalline phases, uniform particle size, ameliorative crystallinity, high surface area and the low mass transfer resistance benefitted from the unique porous structure.

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Facile synthesis of free-standing nickel chalcogenide electrodes for overall water splitting
Haonan Ren, Zheng-Hong Huang, Zhiyu Yang, Shujun Tang, Feiyu Kang, Ruitao Lv
2017 Vol. 26 (6): 1217-1222 [摘要] ( 119 ) [HTML 1KB] [PDF] ( 0 )

Developing high-performance noble metal-free and free-standing catalytic electrodes are crucial for overall water splitting. Here, nickel sulfide (Ni3S2) and nickel selenide (NiSe) are synthesized on nickel foam (NF) with a one-pot solvothermal method and directly used as free-standing electrodes for efficiently catalyzing hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in alkaline solution. In virtue of abundant active sites, the Ni3S2/NF and the NiSe/NF electrodes can deliver a current density of 10 mA cm-2 at only 123 mV, 137 mV for HER and 222 mV, 271 mV for OER. Both of the hierarchical Ni3S2/NF and NiSe/NF electrodes can serve as anodes and cathodes in electrocatalytic overall watersplitting and can achieve a current density of 10 mA cm-2 with an applied voltage of ~1.59 V and 1.69 V, respectively. The performance of as-obtained Ni3S2/NF||Ni3S2/NF is even close to that of the noble metalbased Pt/C/NF||IrO2/NF system.

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CoP nanoparticles embedded in P and N co-doped carbon as efficient bifunctional electrocatalyst for water splitting
Zeqi Zhou, Nasir Mahmood, Yongchao Zhang, Lun Pan, Li Wang, Xiangwen Zhang, Ji-Jun Zou
2017 Vol. 26 (6): 1223-1230 [摘要] ( 124 ) [HTML 1KB] [PDF] ( 0 )

Noble-metal-free hydrogen/oxygen evolution reaction (HER/OER) electrocatalysts, especially bifunctional electrocatalysts, are essential for overall water splitting, but their performance is impeded by many factors like poor electrical conductivity. Herein, we fabricated cobalt phosphide (CoP) nanoparticles embedded in P and N co-doped carbon (PNC) matrix (CoP@PNC) to fully realize the high activity of CoP by maximizing its conductivity. Simply a carbonization coupled phosphidation approach was utilized where Co ions and organic ligands of Co-MOF were transferred into CoP and P and N co-doped carbon. The synthesized material shows an ideal electrical conductivity, excellent HER (overpotential of -84 mV and -120 mV@10 mA cm-2 in acidic and alkaline medias, respectively) and OER (overpotential of 330 mV@10 mA cm-2 in alkaline media) performances. Further, CoP@PNC acts as a superior catalyst for both anode and cathode to catalyze overall water splitting and only requires an voltage of 1.52 V to deliver a current density of 10 mA cm-2, superior to the noble-metal catalysts system (Pt/C//IrO2) and the reported noble-metal-free bifunctional electrocatalysts.

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Hydrogen evolution-assisted one-pot aqueous synthesis of hierarchical trimetallic PdNiRu nanochains for hydrazine oxidation reaction
Tao Yuan, Aijun Wang, Keming Fang, Zhigang Wang, Jiuju Feng
2017 Vol. 26 (6): 1231-1237 [摘要] ( 121 ) [HTML 1KB] [PDF] ( 0 )

A hydrogen evolution-assisted one-pot aqueous approach was developed for facile synthesis of trimetallic PdNiRu alloy nanochain-like networks (PdNiRu NCNs) by only using KBH4 as the reductant, without any specific additive (e.g. surfactant, polymer, template or seed). The products were mainly investigated by transmission electron microscopy (TEM), X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The hierarchical architectures were formed by the oriented assembly growth and the diffusioncontrolled deposition in the presence of many in-situ generated hydrogen bubbles. The architectures had the largest electrochemically active surface area (ECSA) of 84.32 m2 gPd-1 than PdNi nanoparticles (NPs, 65.23 m2 gPd-1), PdRu NPs (23.12 m2 gPd-1), NiRu NPs (nearly zero), and commercial Pd black (6.01 m2 gPd-1), outperforming the referenced catalysts regarding the catalytic characters for hydrazine oxygen reaction (HOR). The synthetic route provides new insight into the preparation of other trimetallic nanocatalysts in fuel cells.

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A general strategy to the synthesis of carbon-supported PdM (M=Co, Fe and Ni) nanodendrites as high-performance electrocatalysts for formic acid oxidation
Yanrong Ma, Tongfei Li, Hao Chen, Xiaojie Chen, Sihui Deng, Lin Xu, Dongmei Sun, Yawen Tang
2017 Vol. 26 (6): 1238-1244 [摘要] ( 133 ) [HTML 1KB] [PDF] ( 0 )

Rational synthesis of a new class of electrocatalysts with high-performance and low-cost is of great significance for future fuel cell devices. Herein, we demonstrate a general one-step simultaneous reduction method to prepare carbon-supported PdM (M=Co, Fe, Ni) alloyed nanodendrites with the assistance of oleylamine and octadecylene. The morphology, structure and composition of the obtained PdM nanodendrites/C catalysts have been fully characterized. The combination of the dendritic structural feature and alloyed synergy offer higher atomic utilization efficiency, excellent catalytic activity and enhanced stability for the formic acid oxidation reaction (FAOR). Strikingly, the as-synthesized PdCo nanodendrites/C catalyst could afford a mass current density of 2467.7 A g-1, which is almost 3.53 and 10.4 times higher than those of lab-made Pd/C sample (698.3 A g-1) and commercial Pd/C catalyst (237.6 A g-1), respectively. Furthermore, the PdCo nanodendrites/C catalyst also exhibit superior stability relative to the Pd/C catalysts, make it a promising anodic electrocatalyst in practical fuel cells in the future. Additionally, the present feasible synthetic approach is anticipated to provide a versatile strategy toward the preparation of other metal alloy nanodendrites/carbon nanohybrids.

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Highly active electrocatalysis of hydrogen evolution reaction in alkaline medium by Ni-P alloy:A capacitance-activity relationship
Chao Cheng, Syed Shoaib Ahmad Shah, Tayyaba Najam, Ling Zhang, Xueqiang Qi, Zidong Wei
2017 Vol. 26 (6): 1245-1251 [摘要] ( 117 ) [HTML 1KB] [PDF] ( 0 )

Different weights of amorphous Ni-P alloy with same P contents were electrodeposited on nickel plate with same area used as cathode for hydrogen evolution reaction (HER). The amorphous Ni-P alloy coatings were characterized for their surface morphology and composition through Scanning electron microscopy (SEM) and Energy dispersive X-ray spectroscopy (EDS) techniques, X-ray photoelectron spectroscopy (XPS) and X-ray diffraction (XRD) analysis. The electrocatalytic activity for HER in alkaline medium is determined by linear scan voltammetry (LSV) and a relationship between HER activity and capacitance is established. The capacitance varies with the loading of the Ni-P on Ni plate but the activity for HER is directly proportional to the capacitance in alkaline and vice versa. 3#Ni-P/Ni containing 3.85 mg Ni-P alloy with highest capacitance performs the best catalytic activity. This work provides direct evidence to explore the capacitance influence on the electrocatalystic activity for the HER.

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Electrodeposited NiSe2 on carbon fiber cloth as a flexible electrode for high-performance supercapacitors
Quanlin Bao, Jihuai Wu, Leqing Fan, Jinhua Ge, Jia Dong, Jinbiao Jia, Jiali Zeng, Jianming Lin
2017 Vol. 26 (6): 1252-1259 [摘要] ( 111 ) [HTML 1KB] [PDF] ( 0 )

A flexible electrode of nickel diselenide/carbon fiber cloth (NiSe2/CFC) is fabricated at room temperature by a simple and efficient electrodeposition method. Owing to NiSe2 character of nanostructure and high conductivity, the as-synthesized electrodes possess perfect pseudocapacitive property with high specific capacitance and excellent rate capability. In three-electrode system, the electrode specific capacitance of the NiSe2/CFC electrode varies from 1058 F g-1 to 996.3 F g-1 at 2 A g-1 to 10 A g-1 respectively, which shows great rate capability. Moreover, the NiSe2 electrode is assembled with an active carbon (AC) electrode to form an asymmetric supercapacitor with an extended potential window of 1.6 V. The asymmetric supercapacitor possesses an excellent energy density 32.7 Wh kg-1 with a power density 800 W kg-1 at the current density of 1 A g-1. The nanosheet array on carbon fiber cloth with high flexibility, specific capacitance and rate capacitance render the NiSe2 to be regarded as the promising material for the high performance superconductor.

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All-solid-state flexible asymmetric supercapacitors with high energy and power densities based on NiCo2S4@MnS and active carbon
Zhiguo Zhang, Xiao Huang, Huan Li, Hongxia Wang, Yingyuan Zhao, Tingli Ma
2017 Vol. 26 (6): 1260-1266 [摘要] ( 114 ) [HTML 1KB] [PDF] ( 0 )

Electrode material based on a novel core-shell structure consisting of NiCo2S4 (NCS) solid fiber core and MnS (MS) sheet shell (NCS@MS) in situ grown on carbon cloth (CC) has been successfully prepared by a simple sulfurization-assisted hydrothermal method for high performance supercapacitor. The synthesized NiCo2S4@MnS/CC electrode shows high capacitance of 1908.3 F g-1 at a current density of 0.5 A g-1 which is higher than those of NiCo2S4 and MnS at the same current density. A flexible all-solid-state asymmetric supercapacitor (ASC) is constructed by using NiCo2S4@MnS/CC as positive electrode, active carbon/CC as negative electrode and KOH/poly (vinyl alcohol) (PVA) as electrolyte. The optimized ASC shows a maximum energy density of 23.3 Wh kg-1 at 1 A g-1, a maximum power density of about 7.5 kw kg-1 at 10 A g-1 and remarkable cycling stability. After 9000 cycles, the ASC still exhibited 67.8% retention rate and largely unchanged charge/discharge curves. The excellent electrochemical properties are resulted from the novel core-shell structure of the NiCo2S4@MnS/CC electrode, which possesses both high surface area for Faraday redox reaction and superior kinetics of charge transport. The NiCo2S4@MnS/CC electrode shows a promising potential for energy storage applications in the future.

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Application of diatomite as an effective polysulfides adsorbent for lithium-sulfur batteries
Zhong Li, Nan Zhang, Yubao Sun, Hanzhong Ke, Hansong Cheng
2017 Vol. 26 (6): 1267-1275 [摘要] ( 106 ) [HTML 1KB] [PDF] ( 0 )

The lithium-sulfur batteries show the great potential to be the most promising candidate for high energy applications. However, the shuttling of soluble polysulfides deteriorates the battery performance tremendously. To suppress the diffusion of soluble polysulfides, diatomite that has abundant natural three-dimensional ordered pores is incorporated into the cathode to trap polysulfides. The composite cathode material (S-DM-AB for short), including sulfur (S), diatomite (DM), and acetylene black (AB) is prepared by an impregnation method. For comparison, another composite cathode material (S-AB for short) including sulfur and acetylene black is also prepared by the same method. The battery with S-DMAB composite cathode material delivers a discharge capacity of 531.4 mAh/g after 300 cycles at 2 C with a capacity retention of 51.6% at room temperature. By contrast, the battery with S-AB composite cathode material delivered a capacity of only 196.9 mAh/g with a much lower capacity retention of 18.6% under the same condition. The addition of diatomite in the cathode is proved to be a cheap and effective way to improve the life time of the lithium sulfur batteries.

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Enhanced cycle performance of Li/S battery with the reduced graphene oxide/activated carbon functional interlayer
Haipeng Li, Liancheng Sun, Yongguang Zhang, Taizhe Tan, Gongkai Wang, Zhumabay Bakenov
2017 Vol. 26 (6): 1276-1281 [摘要] ( 105 ) [HTML 1KB] [PDF] ( 0 )

The high-energy lithium/sulfur (Li/S) battery has become a very popular topic of research in recent years due to its high theoretical capacity of 1672 mAh/g. However, the polysulfide shuttle effect remains of great concern with a great number of publications dedicated to its mitigation. In this contribution, a three-dimensional (3D) reduced graphene oxide/activated carbon (RGO/AC) film, synthesized by a simple hydrothermal method and convenient mechanical pressing, is sandwiched between the separator and the sulfur-based cathode, acting as a functional interlayer to capture and trap polysulfide species. Consequently, the Li/S cell with this interlayer shows an impressive initial discharge capacity of 1078 mAh/g and a reversible capacity of 655 mAh/g even after 100 cycles. The RGO/AC interlayer impedes the movement of polysulfide while providing unimpeded channels for lithium ion mass transfer. Therefore, the RGO/AC interlayer with a well-designed structure represents strong potential for high-performance Li/S batteries.

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Nitrogen-doped hierarchical porous carbon derived from metal-organic aerogel for high performance lithium-sulfur batteries
Han Zhang, Zongbin Zhao, Yang Liu, Jingjing Liang, Yanan Hou, Zhichao Zhang, Xuzhen Wang, Jieshan Qiu
2017 Vol. 26 (6): 1282-1290 [摘要] ( 119 ) [HTML 1KB] [PDF] ( 0 )

Nitrogen-doped three-dimensional (3D) porous carbon materials have numerous applications due to their highly porous structures, abundant structural nitrogen heteroatom decoration and low densities. Herein, nitrogen doped hierarchical 3D porous carbons (NHPC) were prepared via a novel metal-organic aerogel (MOA), using hexamethylenetetramine (HMT), 1,3,5-benzenetricarboxylic acid and copper (Ⅱ) as starting materials. The morphology, porous structure of the building blocks in the NHPC can be tuned readily using different amount of HMT, which makes elongation of the pristine octahedron of HKUST-1 to give rise to different aspect ratio rod-like structures. The as-prepared NHPC with rod-like carbons exhibit high performance in lithium sulfur battery due to the rational ion transfer pathways, high N-doped doping and hierarchical porous structures. As a result, the initial specific capacity of 1341 mA h/g at rate of 0.5 C (1 C=1675 mA h/g) and high-rate capability of 354 mA h/g at 5 C was achieved. The decay over 500 cycles is 0.08% per cycle at 1 C, highlighting the long-cycle Li-S batteries.

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双月刊
(创刊 1992)
2013年由JNGC更名为JEC

ISSN 2095-4956
CN 10-1287/O6

主编
Xinhe Bao
Gabriele Centi


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