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Nano-Au-decorated hierarchical porous cobalt sulfide derived from ZIF-67 toward optimized oxygen evolution catalysis:Important roles of microstructures and electronic modulation

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Carbon Energy 2024年第5期6卷 1-14页

作者： Hongyu Gong Guanliang Sun Wenhua Shi Dongwei Li Xiangjun Zheng Huan Shi Xiu Liang Ruizhi Yang Changzhou Yuan Department of New Energy Materials School of Environmental and Chemical EngineeringJiangsu University of Science and TechnologyZhenjiangJiangsuChina Advanced Materials Institute Qilu University of Technology(Shandong Academy of Sciences)JinanShandongChina Shandong Saikesaisi Hydrogen Energy Co. Ltd.JinanShandongChina Department of Materials Science and Engineering School of Materials Science&EngineeringUniversity of JinanJinanShandongChina Department of New Energy Science and Engineering College of EnergySoochow Institute for Energy and Materials InnovationsSoochow UniversitySuzhouJiangsuChina

Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.

关键词： Au nanoparticles cobalt sulfide electronic modulation hierarchical porous structure oxygen evolution reaction

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Mn-doping induced electronic modulation and rich oxygen vacancies on vertically grown NiFe2O4 nanosheet array for synergistically triggering oxygen evolution reaction

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Nano Research 2022年第5期15卷 3940-3945页

作者： Yonghao Gan Meilin Cui Xiaoping Dai Ying Ye Fei Nie Ziteng Ren Xueli Yin Baoqiang Wu Yihua Cao Run Cai Xin Zhang State Key Laboratory of Heavy Oil Processing College of Chemical Engineering and EnvironmentChina University of PetroleumBeijing 102249China

Large-scale electrolysis of water to produce high-purity hydrogen is one of the effective ways to solve the energy crisis and environmental pollution problems.However,efficient,cheap and stable catalysts are one of the bottlenecks for industrial application in water splitting.Herein,a facile one-step hydrothermal process was applied to fabricate Mn-doped nickel ferrite nanosheets(Mn-NiFe_(2)O_(4))which shown a low overpotential of 200 mV at 50 mA·cm^(-2)and a small Tafel slope of 47 mV·dec^(-1),together with a prominent turnover frequency(TOF)value(0.14 s^(-1))and robust stability.The in-situ UV-vis spectroscopy unveiled the surface reconstruction to generate NiOOH as active sites during oxygen evolution reaction(OER).The excellent electrocatalytic activity of Mn-NiFe_(2)O_(4)is attributed to the vertically grown nanosheets for exposure more active sites,rich oxygen vacancies,and the hybridization between Ni 3d and O 2p orbitals caused by Mn doping.This work should provide a facile strategy by Mn-doping to simultaneously engineer oxygen vacancies and electronic structure for synergistically triggering oxygen evolution reaction.

关键词： Mn doping NiFe_(2)O_(4)nanosheets oxygen vacancies electronic modulation oxygen evolution reaction

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electronic modulation and interface engineering of electrospun nanomaterials‐based electrocatalysts toward water splitting

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Carbon Energy 2021年第1期3卷 101-128页

作者： Wei Song Meixuan Li Ce Wang Xiaofeng Lu State Key Laboratory of Supramolecular Structure and Materials Institute of Theoretical ChemistryCollege of ChemistryJilin UniversityChangchunPeople's Republic of China Alan G.MacDiarmid Institute College of ChemistryJilin UniversityChangchunPeople's Republic of China

Nowdays,electrocatalytic water splitting has been regarded as one of the most efficient means to approach the urgent energy crisis and environmental issues.However,to speed up the electrocatalytic conversion efficiency of their half reactions including hydrogen evolution reaction(HER)and oxygen evolution reaction(OER),electrocatalysts are usually essential to reduce their kinetic energy barriers.Electrospun nanomaterials possess a unique one‐dimensional structure for outstanding electron and mass transportation,large specific surface area,and the possibilities of flexibility with the porous feature,which are good candidates as efficient electrocatalysts for water splitting.In this review,we focus on the recent research progress on the electrospun nanomaterials‐based electrocatalysts for HER,OER,and overall water splitting reaction.Specifically,the insights of the influence of the electronic modulation and interface engineering of these electrocatalysts on their electrocatalytic activities will be deeply discussed and highlighted.Furthermore,the challenges and development opportunities of the electrospun nanomaterials‐based electrocatalysts for water splitting are featured.Based on the achievements of the significantly enhanced performance from the electronic modulation and interface engineering of these electrocatalysts,full utilization of these materials for practical energy conversion is anticipated.

关键词： electrocatalysis electronic modulation electrospun nanomaterials interface engineering water splitting

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In situ growth of NiSe@Co_(0.85)Se heterointerface structure with electronic modulation on nickel foam for overall water splitting

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Rare Metals 2021年第6期40卷 1373-1382页

作者： Wen-Long Ding Yan-Hui Cao Hui Liu Ao-Xuan Wang Cui-Juan Zhang Xue-Rong Zheng Key Laboratory for Green Chemical Technology of Ministry of Education State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China Department of Physics and Astronomy University of CaliforniaIrvineCA 92697USA Tianjin Kaben New Materials Technology Co. Ltd.Tianjin 300350China

Constructing heterointerface engineering has becoming an effective and general strategy for developing highly efficient and durable nonnoble electrocatalysts for catalyzing both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this work,we synthesized a self-supporting heterogeneous NiSe@Co_(0.85)Se/NF electrocatalyst using a facile in situ selenization of transition metal precursors that coated on the nickel foam(NF)in polyol solution.The NF was used as both conductive substrate and nickel source,ensuring superior electronic conductivity for catalyzing.The NiSe@-Co_(0.85)Se/NF exhibited remarkable bifunctional electrocatalytic activities with HER overpotential of 168 mV and OER overpotential of 258 mV to achieve 10 mA·cm-2.The water splitting system using NiSe@Co_(0.85)Se/NF as both anode and cathode electrodes achieved a current density of 10 mA·cm^(-2) at 1.61 V with nearly 100% faradaic efficiency and impressively long-term stability.The efficient bifunctional catalytic performance of NiSe@-Co_(0.85)Se/NF should be attributed to the electronic modulation and synergistic effect between NiSe and Co_(0.85)Se,the intrinsic metallic conductivity and the enlarged active sites exposure.This work provides a facile method for developing heterogeneous bifunctional catalysts for advanced electrochemical energy conversion technologies.

关键词： NiSe@Co_(0.85)Se/NF Heterointerface structure electronic modulation Bifunctional electrocatalyst Overall water splitting

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通过与钌合金化来调控铂的电子结构促进以水为质子源的光催化选择性加氢

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Science China Materials 2024年第3期67卷 824-832页

作者：施曼曼罗点吴鹏沈娅蓉魏杰顶郭赛雅陆洲黄玉成倪永红 College of Chemistry and Materials Science Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecule-Based MaterialsAnhui Key Laboratory of Functional Molecular SolidsAnhui Normal University School of Physics and electronic Information Anhui Normal University

调控金属活性位点的电子结构来发展高活性的选择性加氢反应催化剂对于可持续有机合成非常重要.但时至今日,这仍然是非常具有挑战性的课题.在本文中,我们将具有电子结构调节特性的超细PtRu合金纳米颗粒负载在CdS纳米棒上,成功构建了PtRu/... 详细信息

调控金属活性位点的电子结构来发展高活性的选择性加氢反应催化剂对于可持续有机合成非常重要.但时至今日,这仍然是非常具有挑战性的课题.在本文中,我们将具有电子结构调节特性的超细PtRu合金纳米颗粒负载在CdS纳米棒上,成功构建了PtRu/CdS复合催化剂并研究了其光催化芳香族硝基化合物氢化还原性能.我们发现当以水为质子源时,所得复合催化剂表现出高效的光催化加氢活性.超快光谱研究和密度泛函理论计算揭示了合金的形成促进了光生载流子的分离并降低了氢化还原反应中决速步的能垒,从而显著提高了加氢活性.本研究通过合金化效应调节助催化剂的电子结构,为高活性助催化剂/光催化剂体系的理性设计开辟了一条新途径.

关键词： electronic modulation alloying carrier dynamics photocatalysis nitroaromatic hydrogenation

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Boron modulating electronic structure of FeN4C to initiate high-efficiency oxygen reduction reaction and high-performance zinc-air battery

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Journal of Energy Chemistry 2022年第3期31卷 514-524,I0014页

作者： Xue Zhao Xue Li Zenghui Bi Yuwen Wang Haibo Zhang Xiaohai Zhou Quan Wang Yingtang Zhou Huaisheng Wang Guangzhi Hu Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental ScienceYunnan UniversityKunming 650504YunnanChina College of Chemistry and Molecular Sciences Wuhan UniversityWuhan 430072HubeiChina National Engineering Research Center for Marine Aquaculture Marine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004ZhejiangChina School of Chemistry and Chemical Engineering Liaocheng UniversityLiaocheng 252000ShandongChina

The biggest challenge is to develop a low cost and readily available catalyst to replace expensive commercial Pt/C for efficient electrochemical oxygen reduction reaction(ORR).In this research,closo-[B_(12)H_(12)]^(2−)and 1,10-phenanthroline-iron complexes were introduced into the porous metal-organic framework by impregnation method,and further annealing treatment achieved the successful anchoring of single-atom-Fe in B-doped CN Matrix(FeN4CB).The ORR activity of FeN4CB is comparable to the widely used commercial 20 wt%Pt/C.Where the half-wave potential(E_(1/2))in alkaline medium up to 0.84 V,and even in the face of challenging ORR in acidic medium,the E_(1/2)of ORR driven by FeN4CB is still as high as 0.81 V.When FeN4CB was used as air cathode,the open circuit voltage of Zn-air battery reaches 1.435 V,and the power density and specific capacity are as high as 177 mW cm^(−2)and 800 mAh g_(Zn)^(−1)(theoretical value:820 mAh g_(Zn)^(−1)),respectively.The dazzling point of FeN4CB also appears in the high ORR stability,whether in alkaline or acidic media,E_(1/2)and limiting current density are still close to the initial value after 5000 times cycles.After continuously running the charge-discharge test for 220 h,the charge voltage and discharge voltage of the rechargeable zinc-air battery with FeN4CB as the air cathode maintained the initial state.Density functional theory calculations reveals that introducing B atom to Fe–N4–C can adjust the electronic structure to easily break O=O bond and significantly reduce the energy barrier of the rate-determining step resulting in an improved ORR activity.

关键词： Single-atom Fe B-doped CN Oxygen reduction reaction Zn-air battery electronic modulation

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Nest-type NCM ■ Pt/C with oxygen capture character as advanced electrocatalyst for oxygen reduction reaction

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Journal of Energy Chemistry 2022年第8期31卷 304-312,I0009页

作者： Teng Chen Yida Xu Deming Meng Xuefeng Guo Yan Zhu Luming Peng Jianqiang Hu Weiping Ding Key Lab of Mesoscopic Chemistry School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023JiangsuChina Department of Aviation Oil and Material Air Force Logistics AcademyXuzhou 221000Jiangsu.China

A unique nest-type catalyst has been designed with a nest of oxygen capture surrounding catalytic Pt centers, which shows much promoted performance, on the base of Pt/C catalyst, for oxygen reduction reaction(ORR). The nest is constructed with nitrogen-doped carbon matrix(NCM), derived from the controlled carbonization of PANI precursor, to cover Pt/C catalyst. The unique structure of the catalyst(denoted as NCM■ Pt/C) has many merits. Firstly, it can capture oxygen both in air and in acidic electrolyte. Compared with naked Pt/C, it is found that, in air, the oxygen concentration within the porous nest of NCM surrounding Pt/C particles is ~13 times higher than atmospheric oxygen concentration and, in acidic electrolyte, the concentration of activated oxygen over the catalyst NCM■ Pt/C rise to~1.9 times. Secondly, the NCM nest offers a special electronic modulation on Pt centers toward modified ORR kinetics and then catalytic performances. With these merits, compared with Pt/C, the NCM■ Pt/C catalyst shows 3.2 times higher turnover frequency value and 2.9 times enhanced specific activity for ORR with half-wave potential at 0.894 V. After 50,000 sweeping cycles, the NCM■ Pt/C catalyst retains~66% mass activity and still has advantages over the fresh Pt/C catalyst. We envision that the nest-type catalyst provides a new idea for progress of practical Pt/C ORR catalyst.

关键词： Oxygen reduction reaction Surrounding environment Nest-type catalyst Oxygen capture electronic modulation

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通过阴、阳离子取代调控Ni_(2)P的电子结构用于高效氧析出反应

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Science China Materials 2022年第6期65卷 1522-1530页

作者：张珂新张子韬沈昊明唐彦群梁子彬邹如强 Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials School of Materials Science and EngineeringPeking UniversityBeijing 100871China Institute of Clean Energy Peking UniversityBeijing 100871China

合理设计具有结构和组分优势的氧析出反应(OER)催化剂对电催化能源转换技术至关重要.过渡金属磷化物是较有前景的OER催化剂.将杂原子引入过渡金属磷化物的晶格可以引起晶格畸变和电子密度的重新分布,从而改变电子结构,提高催化性能.在... 详细信息

合理设计具有结构和组分优势的氧析出反应(OER)催化剂对电催化能源转换技术至关重要.过渡金属磷化物是较有前景的OER催化剂.将杂原子引入过渡金属磷化物的晶格可以引起晶格畸变和电子密度的重新分布,从而改变电子结构,提高催化性能.在此基础上,本文通过部分硫化和随后的磷化过程,将预先合成的镍铁金属有机框架(NiFe-MOFs)转化为均匀分散在多孔碳基底上的Fe和S取代的Ni_(2)P(Ni–Fe–P–S@C).实验结果和密度泛函理论计算表明,Fe和S的掺入可以调节Ni_(2)P的电子结构,改变反应中间体的吸附自由能,使得Ni–Fe–P–S@C具有良好的OER催化活性和稳定性.值得注意的是,原位形成的部分氧化的表面对改善局部环境并进一步提升催化活性至关重要.本文提出的阴、阳离子取代策略为提高过渡金属基催化剂的电催化性能带来了新的启示.

关键词： oxygen evolution reaction electrocatalysis transition-metal phosphide cation-and anion-substitution electronic modulation

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Bioinspired Construction of Ruthenium-decorated Nitrogen-doped Graphene Aerogel as an Efficient Electrocatalyst for Hydrogen Evolution Reaction

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Chemical Research in Chinese Universities 2020年第4期36卷 709-714页

作者： SHI Yi DAI Wenru WANG Meng XING Yongfang XIA Xinghua CHEN Wei Department of Chemistry National University of Singapore3 Science Drive 3117543Singapore State Key Laboratory of Analytical Chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023P.R.China National University of Singapore(Suzhou)Research Institute Suzhou 215123P.R.China Joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityBinhai New CityFuzhou 350207P.R.China Department of Physics National University of Singapore117542Singapore

Rational construction of low-cost,efficient,and durable electrocatalysts for the hydrogen evolution reac-tion(HER)is essential to further develop water electrolysis industry.Inspired by the natural enzyme catalysis with coordination environments of catalvtic sites and three-dimensional structures.we construct an efficient Ru-based catalyst anchored on the nitrogen dopant on graphene aerogel(Ru-NGA).The Ru-NGA catalyst exhibits dramatically improved electroactivity and stability towards HER with a near-zero onset overpotential,a low Tafel slope of 32mVidec,and a high turnover frequency of 5.5 s^-1 at-100 mV.The results show that the electronic modulation of metallic Ru nanoparticles by nitrogen coordination weakens the affinity of Ru towards H and hence facilitates the de.sorption of hydrogen.This research provides in-depth insights into the fundamental relationship between metallic nanostructure and HER activity,and also guides the rational design of high-performance electrocatalysts in energy conversion.

关键词： Ruthenium Graphene aerogel Hydrogen evolution reaction electronic modulation Electrocatalysis

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