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Nano Research 2018年第4期11卷 2149-2158页

作者： Jiahao Yu gongzhen cheng Wei Luo College of Chemistry andMolecularSciences Wuhan University Wuhan 430072 China Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China

The development of efficient and stable non-noble metal-based electrocatalysts for the oxygen evolution reaction （OER） is one of the essential challenges for the upcoming hydrogen economy. Herein, three-dimensional （3D） mesoporous nickel iron selenide with rose-like microsphere architecture was directly grown on Ni foam via a successive two-step hydrotherrnal method. The unique 3D mesoporous rose-like morphology leads to a higher number of active sites as well as fast mass and electron transport through the entire electrode, and facilitates the release of 02 bubbles formed during the OER catalysis. As a result, the synthesized Ni0.76Fe0.24Se exhibits superior OER performances, with an ultralow overpotential of 197 mV needed to produce a current density of 10 ***-2 in 1 M KOH, outperforming all transition metal selenide OER catalysts reported to date.

关键词： transition metal selenide oxygen evolution reaction NiFeSe three-dimensional (3D) rose-like microspheres

Nitrogen-doped graphene hydrogel-supported NiPt-CeOx nanocomposites and their superior catalysis for hydrogen generation from hydrazine at room temperature

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Nano Research 2017年第8期10卷 2856-2865页

作者： Xiaoqiong Du Chao Liu cheng Du Ping Cai gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences Wuhan University Wuhan 430072 China Key laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University Tianjin 300071 China

The safe and efficient storage and release of hydrogen is one of the key technological challenges for the fuel cell-based hydrogen economy. Hydrazine monohydrate has attracted considerable attention as a safe and convent chemical hydrogen-storage material. Herein, we report the facile synthesis of NiPt-CeOx nanocomposites supported by three-dimensional nitrogen-doped graphene hydrogels （NGHs） via a simple one-step co-reduction synthesis method. These catalysts were composition-dependent for hydrogen generation from an alkaline solution of hydrazine. （NisPt5）I-（CeOx）0.B/NGH exhibited the highest catalytic activity, with 100% hydrogen selectivity and turnover frequencies of 408 h^-1 at 298 K and 3,064 h^-1 at 323 K. These superior catalytic performances are attributed to the electronic structure of the NiPt centers, which was modified by the electron interaction between NiPt and CeOx and the strong metal-support interaction between NiPt-CeOx and the NGH.

关键词： nitrogen-doped graphene hydrogels NiPt-CeOx hydrogen storage hydrazine

NiRh nanoparticles supported on nitrogen-doped porous carbon as highly efficient catalysts for dehydrogenation of hydrazine in alkaline solution

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Nano Research 2015年第11期8卷 3472-3479页

作者： Bingquan Xia Kang Chen Wei Luo gongzhen cheng College of Chemistry and Molecular Sciences Wuhan University Wuhan Hubei 430072 China Suzhou Institute of Wuhan University Suzhou Jiangsu 215123 China

Well-dispersed bimetallic NiRh nanoparticles （NPs） with different compositions supported on nitrogen-doped porous carbon （NPC） derived from metal-organic frameworks （ZIF-8） were synthesized through a co-reduction method. The NPC-900 supported NiRh catalyst exhibits the highest catalytic activity and 100% hydrogen selectivity toward hydrogen generation from hydrazine. These properties might be attributed to the high surface area and high graphitization of the NPC. This strategy may open up a new avenue for designing high-performance catalysts by utilizing NPC as a support to anchor active metal NPs for additional applications.

关键词： hydrogen storage metal--organic frameworks nitrogen-doped porous carbon hydrazine

Nickel-iron borate coated nickel-iron boride hybrid for highly stable and active oxygen evolution electrocatalysis

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Chinese Chemical Letters 2020年第9期31卷 2469-2472页

作者： Pengyu Han Tan Tan Fei Wu Ping Cai gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China Department of Orthopaedic Surgery Renmin Hospital of Wuhan UniversityWuhan 430060China Suzhou Institute of Wuhan University Suzhou 215123China

The development of efficient and cost-effective electrocatalysts toward anodic oxygen evolution reaction(OER) is crucial for the commercial application of electrochemical water *** the most promising electrocatalysts,the OER performances of nickel-iron-based materials can be further improved by introducing metalloid elements to modify their electron ***,we developed an efficient hybrid electrocatalyst with nickel-iron boride(NiFeB) as core and amorphous nickel-iron borate(NiFeBi)as shell(NiFeB@NiFeBi) via a simple aqueous *** obtained NiFeB@NiFeBi exhibits a small overpotential of 237 mV at 10 mA/cm^2 and Tafel slope of 57.65 mV/dec in 1.0 mol/L KOH,outperforming most of the documented precious-metal-free based *** from the in situ formed amorphous NiFeBi layer,it shows excellent stability toward the oxygen evolution reaction(OER).These findings might provide a new way to design advanced precious-metal-free electrocatalysts for OER and the application of electrochemical water splitting.

关键词： Oxygen evolution reaction Metal boride Metal borate Core-shell

The Role of Hydroxide Binding Energy in Alkaline Hydrogen Oxidation Reaction Kinetics on RuCr Nanosheet

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Chinese Journal of Chemistry 2022年第21期40卷 2495-2501页

作者： Chaoyi Yang Yunbo Li Chuangxin Ge Wenyong Jiang gongzhen cheng Lin Zhuang Wei Luo College of Chemistry and Molecular Sciences Wuhan UniversityWuhanHubei 430072China Hubei Key Labon Organic and Polymeric Opto-Electronic Materials Wuhan UniversityWuhanHubei 430072China

Unveiling the role of adsorbed hydroxide involved in the hydrogen oxidation reaction(HOR)under alkaline electrolyte is crucial for the development of advanced HOR electrocatalysts for the alkaline polymer electrolyte fuel cells(APEFCs).Herein,we report the synthesis of amorphous RuCr nanosheets with different molar ratios and their HOR performances under alkaline *** find a volcano correlation between the Cr content in RuCr nanosheets and their alkaline HOR *** results and density functional theory(DFT)calculation reveals that the optimized Cr content in RuCr nanosheets could lead to the optimum hydroxide binding energy(OHBE),contributes to their remarkable alkaline HOR performance with mass activity of 568.1 A·gPGM^(–1) at 50 mV,13-fold higher than that of Ru *** RuCr nanosheet is further used as the anodic electrocatalyst,a peak power density of 1.04 W·cm^(–2 )can be achieved in an APEFC.

关键词： Fuel cells Hydrogen oxidation reaction Hydroxide binding energy Electrochemistry Ruthenium

Molybdenum-induced tuning 3d-orbital electron filling degree of CoSe_(2) for alkaline hydrogen and oxygen evolution reactions

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Chinese Chemical Letters 2023年第2期34卷 274-278页

作者： Sumaira Nazar Hussain Yana Men Zhen Li Pingping Zhao gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China School of Printing and Packaging Wuhan UniversityWuhan 430072China Suzhou Institute of Wuhan University Suzhou 215123China

The development of high-performance non-precious metal-based robust bifunctional electrocatalyst for both hydrogen evolution reaction(HER) and oxygen evolution reactions(OER) in alkaline media is essential for the electrochemical overall water splitting technologies. Herein, we demonstrate that the HER/OER performance of Co Se_(2)can be significantly enhanced by tuning the 3d-orbital electron filling degree through Mo doping. Both density functional theory(DFT) calculations and experimental results imply that the doping of Mo with higher proportion of the unoccupied d-orbital(P_(un)) could not only serve as the active center for water adsorption to enhance the water molecule activation, but also modulate the electronic structures of Co metal center leading to the optimized adsorption strength of*H. As expected, the obtained Mo-Co Se_(2)exhibits a remarkable bifunctional performance with overpotential of only 85 m V for HER and 245 m V for OER to achieve the current density of 10 m A/cm^(2)in alkaline *** work will provide a valuable insight to design highly efficient bifunctional electrocatalyst towards HER and OER.

关键词： Alkaline HER OER Cobalt selenide Proportion of unoccupied d-orbital(Pun) 3d-orbital electron filling degree DFT

NiPt nanoparticles supported on CeO_2 nanospheres for efficient catalytic hydrogen generation from alkaline solution of hydrazine

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Chinese Chemical Letters 2019年第3期30卷 634-637页

作者： Yana Men Jun Su Xiangli Wang Ping Cai gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences Wuhan University Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology No.1 Middle School Affiliated to Central China Normal University

Searching for highly efficient catalysts toward dehydrogenation of hydrazine for chemical hydrogen storage is highly desirable for the development of hydrogen economy. Herein, we report a simple in situ co-reduction synthesis of NiPt nanoparticles supported on CeO_2 nanospheres and their superior catalytic performance for hydrogen generation from alkaline solution of hydrazine at room temperature. Thanks to the strong electronic interaction arising from synergistic effect at atomic lever and support-metal interaction between NiPt and CeO_*** obtained Ni_5Pt_5-CeO_2 catalyst exhibits 100% hydrogen selectivity and superior catalytic performance for hydrogen generation from alkaline solution of hydrazine at room temperature, with a TOF value of 416 h 1.

关键词： Hydrogen storage Hydrazine Hydrogen evolution CeO2 nanospheres Support-metal in teraction

Enhanced catalytic activity of Ru through N modification toward alkaline hydrogen electrocatalysis

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Chinese Chemical Letters 2022年第2期33卷 1065-1069页

作者： Yuanmeng Zhao Xuewei Wang Zhen Li Pingping Zhao Congliang Tao gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China School of Printing and Packaging Wuhan UniversityWuhan 430072China Wuhan Foreign Language School Wuhan 430022China Suzhou Institute of Wuhan University Suzhou 215123China Yangzhou Kairuite Medical Products Co. Ltd.Yangzhou 225200China

Exploring highly efficient electrocatalysts and understanding the reaction mechanisms for hydrogen electrocatalysis,including hydrogen oxidation reaction (HOR) and hydrogen evolution reaction (HER) in alkaline media are conducive to the conversion of hydrogen ***,we reported a new strategy to boost the HER/HOR performances of ruthenium (Ru) nanoparticles through nitrogen (N) *** obtained N-Ru/C exhibit remarkable catalytic performance,with normalized HOR exchange current density and mass activity of 0.56 m A/cm^(2)and 0.54 m A/μg,respectively,about 4 and 4.5 times higher than those of Ru/C,and even twofold enhancement compared to commercial Pt/***,at the overpotential of 50 m V,the normalized HER current density of N-Ru/C is 5.5 times higher than that of Ru/*** and density functional theory (DFT) results verify the electronic regulation of Ru after N incorporation,resulting in the optimized hydrogen adsorption Gibbs free energy (ΔG_(H*)) and hence enhancing the HOR/HER performance.

关键词： Hydrogen oxidation reaction Hydrogen evolution reaction Ru N-incorporation DFT

Three-dimensional nitrogen-doped graphene hydrogel supported Co-CeOx nanoclusters as efficient catalysts for hydrogen generation from hydrolysis of ammonia borane

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Chinese Chemical Letters 2018年第11期29卷 1671-1674页

作者： Yana Men Jun Su Chaozhang Huang Lijing Liang Ping Cai gongzhen cheng Wei Luo College of Chemistry and Molecular Sciences. Wuhan University Wuhon 430072 China Wuhan National Laboratory for Optoelectronics Huazhong University of Science and Technology Wuhan 430074 China Technical Center of Fujian Tobacco Industrial Co. Ltd. Xiamen 361022 China

The development of highly active noble-metal-flee catalysts for catalytic hydrolysis of ammonia borane is mandatory for its application in hydrogen storage. Herein, Co-CeOx nanoclusters have been successfully anchored on a three-dimensional nitrogen-doped graphene hydrogel （NGH） by a simple coreduction method and further used as efficient catalysts to catalytic hydrolysis of ammonia borane at room temperature. Thanks to the strong synergistic electronic effect between Co and CeOx, as well as the strong metal-support interaction between Co-CeOx and 3D NGH, the as-synthesized Co-（CeOx）0.91/NGH catalyst exhibits superior catalytic activity toward hydrolysis of ammonia borane, with the turnover frequency （TOF） value of 79.5 min 1, which is almost 13 times higher than that of Co]NGH, and higher than most of the reported noble-metal-free catalysts.

关键词： Nitrogen-doped graphene hydrogel Co-CeOx Hydrogen storage Ammonia borane Noble-metal-free

A synergy establishment by metal-organic framework and carbon quantum dots to enhance electrochemical water oxidation

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Chinese Chemical Letters 2022年第1期33卷 562-566页

作者： Qiuxiang Mou Xuan Wang Zhenhang Xu Pnur Zul Erlei Li Pingping Zhao Xinghai Liu Houbin Li gongzhen cheng School of Printing and Packaging Wuhan UniversityWuhan 430072China College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072China

Available online Integrating transition metal centered MOFs with conductive materials is a feasible route to enhance electron transfer efficiency of ***,a composite porous structure CQDs_(10)@NiFe-MOF-A was fabricated via introducing carbon quantum dots(CQDs)into porous *** CQDs would make partial loss of lattice in MOF during its growth,leading to the composite building block with the coexistance of crystalline region and amorphous *** calcining treatment would produce an ultrathin protective layer as well as some lattice *** synergy effect between NiFe ions effectively regulated electronic structure of metal active sites,and successful grafting of CQDs to NiFe-MOF significantly improved electrical *** expected,the catalyst exhibited outstanding OER performances with high mass activity of 91.6 A/g at overpotential of 300 mV and robust durability of 10,000 cycles in 1 mol/L KOH,which outperformed that of noble catalyst IrO_(2)of 25.2 A/*** strategy paves a feasible and effective avenue for the non-noble metal catalysts.

关键词： Metal-organic framework Carbon quantum dots Electrochemical impedance spectroscopy Oxygen evolution reaction Stability