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Selectively nucleotide-derived RuP on N,P-codoped carbon with engineered mesopores for energy-efficient hydrogen production assisted by hydrazine oxidation

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SusMat 2024年第1期4卷 166-177页

作者： Xiya Guan Yu Sun Simeng Zhao Haibo Li Suyuan Zeng Qingxia Yao Rui Li Hongyan Chen Konggang Qu School of Chemistry and Chemical Engineering Shandong Provincial Key Laboratory/Collaborative Innovation Center of Chemical Energy Storage&Novel Cell TechnologyLiaocheng UniversityLiaochengChina

Integrating hydrogen evolution reaction(HER)with hydrazine oxidation reaction(HzOR)has an encouraging prospect for the energy-saving hydrogen production,demanding the high-performance bifunctional HER/HzOR electrocatalyst.Ruthenium phosphide/doped carbon composites have exhibited superior activity towardmultiple electrocatalytic reactions.To explore the decent water-soluble precursors containing bothNand P elements is highly attractive to facilely prepare metal phosphide/doped carbon composites.Herein,as one kind ecofriendly biomolecules,adenine nucleotide was first employed to selectively fabricate the highly pure RuP nanoparticles embedded into porous N,P-codoped carbons(RuP/PNPC)with a straightforward“mix-and-pyrolyze”approach.The newly prepared RuP/PNPC only requires 4.0 and−83.0 mV at 10 mA/cm^(2) separately in alkaline HER and HzOR,outperforming most of reported electrocatalysts,together with the outstanding neutral bifunctional performance.Furthermore,the two-electrode alkaline and neutral overall hydrazine splitting both exhibit significant power-efficiency superiority to the corresponding overall water splitting with the voltage difference of larger than 2 V,which can be also easily driven by the fuel cells and solar cells with considerableH2 generation.Our report innovates the N-and P-bearing adenine nucleotide to effortlessly synthesize the high-quality RuP/doped carbon composite catalysts,highly potential as a universal platform for metal phosphide-related functional materials.

关键词： bifunctional electrocatalyst hydrazine oxidation hydrogen energy hydrogen evolution RuP

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Elucidating the electro-catalytic oxidation of hydrazine over carbon nanotube-based transition metal single atom catalysts

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Nano Research 2021年第12期14卷 4650-4657页

作者： Jin Zhang Yaxin Wang Chujie Yang Sian Chen Zhengjian Li Yi Cheng Haining Wang Yan Xiang Shanfu Lu Shuangyin Wang Beijing Key Laboratory of Bio-inspired Energy Materials and Devices&School of Space and Environment Beihang UniversityBeijing100191China Department of Environmental Engineering School of Metallurgy and EnvironmentCentral South UniversityChangsha410083China State Key Laboratory of Chem/Bio-Sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha410082China

Elucidating the reaction mechanism of hydrazine oxidation reaction(HzOR)over carbon-based catalysts is highly propitious for the rational design of novel electrocatalysts for HzOR.In present work,isolated first-row transition metal atoms have been coordinated with N atoms on the graphite layers of carbon nanotubes via a M-N_(4)-C configuration(MSA/CNT,M=Fe,Co and Ni).The HzOR over the three single atom catalysts follows a predominant 4-electron reaction pathway to emit N_(2) and a negligible 1-electron pathway to emit trace of NH3,while their electrocatalytic activity for HzOR is dominated by the absorption energy of N2H4 on them.Furthermore,FeSA/CNT reverses the passivation effect on Fe/C and shows superior performance than CoSA/CNT and NiSA/CNT with a recorded high mass activity for HzOR due to the higher electronic charge of Fe over Co and Ni in the M-N_(4)-C configuration and the lowest absorption energy of N_(2)H_(4) on FeSA/CNT among the three MSA/CNT catalysts.

关键词： hydrazine oxidation single atom catalyst transition metals differential electrochemical mass spectroscopy direct hydrazine fuel cell

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Novel nanoporous binary Ag-Ni electrocatalysts for hydrazine oxidation

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Rare Metals 2010年第1期29卷 26-31页

作者： YI Qingfeng, LI Lei, YU Wenqiang, LIU Xiaoping, ZHOU Zhihua, and NIE Huidong School of Chemistry and Chemical Engineering, Hunan University of Science and Technology, Xiangtan 411201, China School of Chemistry and Chemical Engineering Hunan University of Science and Technology Xiangtan China

From an aqueous mixture of Ag（I）-EDTA complex and Ni（II） nitrate, silver and nickel particles were co-deposited on the surface of titanium substrates by the hydrothermal method using hydrazine hydrate as a reduction agent. The prepared titanium-supported nano-scale Ag and Ag-Ni particles （nano Ag/Ti, nano Ag86Ni14/Ti, nano Ag77Ni23/Ti, and nano Ag74Ni26/Ti） exhibit nanoporous 3D network textures. Their electrocatalytic activity towards hydrazine oxidation in alkaline solutions was evaluated by cyclic voltammetry and chronoamperometry. The results show that the four samples present a low onset potential of ca. -0.60 V vs. SCE and considerably high and stable anodic current densities for hydrazine oxidation. Among them, the nano Ag86Ni14/Ti electrode exhibits the highest anodic current density towards hydrazine oxidation, showing an increment of electro-active sites on the nano Ag86Ni14/Ti due to the addition of Ni to Ag particles.

关键词： electrocatalyst silver hydrazine oxidation fuel cell

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Hierarchical nano-on-micro copper with enhanced catalytic activity towards electro-oxidation of hydrazine

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Frontiers of Materials Science 2018年第1期12卷 45-52页

作者： Xiaodong YAN Yuan LIU Kyle R. SCHEEL Yong LI Yunhua YU Xiaoping YANG Zhonghua PENG Department of Chemistry University of Missouri-Kansas City Kansas City MO 64110 USA State Key Lab of New Ceramics and Fine Processing School of Materials Science and Engineering Tsinghua University Beijing 100084 China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology Beijing 100029 China

The electrochemical properties of catalyst materials are highly dependent on the materials structure and architecture. Herein, nano-on-micro Cu electrodes are fabricated by growing Cu microcrystals on Ni foam substrate, followed by introducing Cu nanocrystals onto the surface of the Cu microcrystals. The introduction of Cu nanocrystals onto the surface of Cu microcrystals is shown to dramatically increase the electrochemically active surface area and thus significantly enhances the catalytic activity of the catalyst electrode towards electro-oxidation of hydrazine. The onset potential （-1.04 V vs. AglAgCI） of the nano-on-micro Cu electrode is lower than those of the reported Cu-based catalysts under similar testing conditions, and a current density of 16 mA-cm-2, which is 2 times that of the microsized Cu electrode, is achieved at a potential of -0.95 V vs. Ag/AgCh Moreover, the nano-on-micro Cu electrode demonstrates good long-term stability.

关键词： electrocatalysis hydrazine oxidation copper nanocrystal hierarchicalarchitecture

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一种用于肼氧化-复合海水电解制氢的富吡啶氮碳纸

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Science China Materials 2024年第3期67卷 752-761页

作者：马闪闪喻博夏宝玉游波 Key Laboratory of Material Chemistry for Energy Conversion and Storage(Ministry of Education) Hubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-80... 详细信息

丰富的中性海水有望替代高纯淡水用于绿氢制备,然而基于过渡金属材料催化的直接海水电解会因析氯反应(ClER)引发严重的腐蚀问题并造成二次重金属污染,且析氧反应(OER)的动力学缓慢.本工作中,我们报道了一种稳定的富吡啶氮的碳纸(N-CP-800),可以有效地催化肼氧化反应(HzOR),以取代中性海水中的OER用于节能制氢.结合电化学实验、原位衰减全反射-表面增强傅里叶变换红外光谱表征和密度泛函理论计算,我们发现:相较于吡咯氮和石墨氮,zig和arm构型的吡啶氮更有利于决速步(^(*)H+N_(2)H_(1))的质子脱附,以促进肼氧化反应.因此,N-CP-800在中性介质中进行HzOR时,仅需0.78 V(相对于可逆氢电势)便可达到10 mA cm^(-2),低于其OER/ClER竞争反应.当N-CP-800与非贵金属析氢催化剂CoP耦合进行HzOR-复合海水电解时,仅需1.56 V的电压即可达到10 mA cm^(-2),并能稳定运行200 h,优于Pt/C和RuO_(2)标准电极对催化的海水电解.

关键词： seawater electrolysis hydrazine oxidation hydrogen evolution nitrogen doping metal-free carbon

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Heteroatom-Induced Accelerated Kinetics on Nickel Selenide for Highly Efficient hydrazine-Assisted Water Splitting and Zn-hydrazine Battery

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Nano-Micro Letters 2023年第9期15卷 492-504页

作者： Hao-Yu Wang Lei Wang Jin-Tao Ren Wen-Wen Tian Ming-Lei Sun Zhong-Yong Yuan School of Materials Science and Engineering Smart Sensing Interdisciplinary Science CenterNankai UniversityTianjin 300350People’s Republic of China Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) Nankai UniversityTianjin 300071People’s Republic of China

hydrazine-assisted water electrolysis is a promising energy conversion technology for highly efficient hydrogen production.Rational design of bifunctional electrocatalysts,which can simultaneously accelerate hydrogen evolution reaction(HER)/hydrazine oxidation reaction(HzOR)kinetics,is the key step.Herein,we demonstrate the development of ultrathin P/Fe co-doped NiSe_(2) nanosheets supported on modified Ni foam(P/Fe-NiSe_(2)) synthesized through a facile electrodeposition process and subsequent heat treatment.Based on electrochemical measurements,characterizations,and density functional theory calculations,a favorable“2+2”reaction mechanism with a two-step HER process and a two-step HzOR step was fully proved and the specific effect of P doping on HzOR kinetics was investigated.P/Fe-NiSe_(2) thus yields an impressive electrocatalytic performance,delivering a high current density of 100 mA cm^(−2) with potentials of−168 and 200 mV for HER and HzOR,respectively.Additionally,P/Fe-NiSe_(2) can work efficiently for hydrazine-assisted water electrolysis and Zn-hydrazine(Zn-Hz)battery,making it promising for practical application.

关键词： Water electrolysis Hydrogen production hydrazine oxidation Bifunctional electrocatalyst Heteroatom doping

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Ru/NC heterointerfaces boost energy-efficient production of green H_(2)over a wide pH range

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Nano Research 2022年第6期15卷 5134-5142页

作者： Qifeng Yang Botao Zhu Feng Wang Cunjin Zhang Jiahao Cai Peng Jin Lai Feng Soochow Institute for Energy and Materials Innovation(SIEMIS) School of EnergySoochow UniversitySuzhou 215006China School of Materials Science and Engineering Hebei University of TechnologyTianjin 300130China

Green hydrogen(H_(2))is an import energy carrier due to the zero-carbon emission in the energy cycle.Nevertheless,green H_(2)production based on electrolyzer and photovoltaics(EZ/PV)remains limited due to the highly pH-dependant and energy exhausting overall water splitting.Herein,we report a series of Ru-nanocluster-modified mesoporous nanospheres(Rux@mONC)as pH-universal electrocatalysts towards both hydrogen evolution reaction(HER)and hydrazine oxidation reaction(HzOR).The optimal catalyst Ru_(2)0@mONC realizes remarkable catalytic activity and stability towards both HER and HzOR regardless of electrolytes.As a result,the electrode pair of Ru_(2)0@mONC//Ru_(2)0@mONC requires low cell-potentials of 39/429,405/926,and 164/1,141 mV to achieve the current density of 10/100 mA·cm^(−2),as well as the long-term stability for HzOR assisted electrochemical water splitting in alkaline,acidic,and neutral media,respectively.Those performances are more promising compared to the state-of-the-art electrocatalysts so far reported.A proof-of-concept test demonstrates an efficient production of green H_(2)powered by a single-junction silicon solar cell,which may inspire the use of a cost-effective EZ/PV system.Furthermore,a combined spectroscopic and theoretical study verifies the formation of abundant Ru/NC heterointerfaces in Ru_(2)0@mONC,which not only contributes to the balancing of H*adsorption/desorption in HER but also facilitates the*N_(2)H_(2)dehydrogenation in HzOR.

关键词： energy-efficient hydrogen production hydrazine oxidation heterointerface dehydrogenation photovoltaicselectrochemistry coupling

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Magic hybrid structure as multifunctional electrocatalyst surpassing benchmark Pt/C enables practical hydrazine fuel cell integrated with energy-saving H_(2)production

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eScience 2022年第4期2卷 416-427页

作者： Ziyun Li Wentao Wang Qizhu Qian Yin Zhu Yafei Feng Yangyang Zhang Huaikun Zhang Mingyu Cheng Genqiang Zhang Hefei National Research Center for Physical Sciences at the Microscale CAS Key Laboratory of Materials for Energy ConversionDepartment of Materials Science and EngineeringUniversity of Science and Technology of ChinaHefeiAnhui230026China Guizhou Provincial Key Laboratory of Computational Nano-Material Science Guizhou Education UniversityGuiyangGuizhou550018China

A hybrid catalyst structure can provide abundant active sites and tailored electronic properties,but the major challenge lies in achieving delicate control over its composition and architecture to improve the catalytic activity toward different electrochemical reactions simultaneously.Herein,we present the rational design of a magic hybrid structure with low Pt loading(5.90 wt%),composed of CoPt_(3)and CoPt nanoparticles supported on N-doped carbon(CoPt_(3)/CoPt⊂PLNC).Importantly,it shows superior multifunctional catalytic activity in alkaline conditions,requiring a low overpotential of 341 and 20 mV to achieve 10 mA cm^(−2)for the hydrazine oxidation reaction(HzOR)/hydrogen evolution reaction(HER),respectively,and it delivers a half-wave potential of 0.847 V for the oxygen reduction reaction(ORR).Theoretical calculations reveal that the metal-carbon hybrid modulates kinetic behavior and induces electron redistribution,achieving the energetic requirements for multiple electrocatalysis.We demonstrate sustainable H_(2)production utilizing solely the CoPt_(3)/CoPt⊂PLNC catalyst,without external electric power input,suggesting its inspiring practical utility.

关键词： Electrocatalysis Hybrid structure Fuel cell hydrazine oxidation H_(2)production

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