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NiSe_(2)-CoSe_(2) with a Hybrid Nanorods and Nanoparticles Structure for Efficient oxygen evolution reaction

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Chinese Journal of Structural Chemistry 2022年第1期41卷 19-24页

作者： Meng Li Ligang Feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225002China

Hetero-structure induced high performance catalyst for oxygen evolution reaction(OER)in the water splitting reaction has received increased attention.Herein,we demonstrated a novel catalyst system of NiSe_(2)-CoSe_(2) consisting of nanorods and nanoparticles for the efficient OER in the alkaline electrolyte.This catalyst system can be easily fabricated via a low-temperature selenization of the solvothermal synthesized NiCo(OH)x precursor and the unique morphology of hybrid nanorods and nanoparticles was found by the electron microscopy analysis.The high valence state of the metal species was indicated by X-ray photoelectron spectroscopy study and a strong electronic effect was found in the NiSe_(2)-CoSe_(2) catalyst system compared to their counterparts.As a result,NiSe_(2)-CoSe_(2) exhibited high catalytic performance with a low overpotential of 250 mV to reach 10 mA·cm^(-2) for OER in the alkaline solution.Furthermore,high catalytic stability and catalytic kinetics were also observed.The superior performance can be attributed to the high valence states of Ni and Co and their strong synergetic coupling effect between the nanorods and nanoparticles,which could accelerate the charge transfer and offer abundant electrocatalytic active sites.The current work offers an efficient hetero-structure catalyst system for OER,and the results are helpful for the catalysis understanding.

关键词： oxygen evolution reaction NiSe_(2) CoSe_(2) hetero-structure electrocatalysis

Revealing component synergy of Ni‒Fe/black phosphorous composites synthesized by self-designed electrochemical method for enhancing photoelectrocatalytic oxygen evolution reaction

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Frontiers of Materials Science 2023年第2期17卷 143-153页

作者： He Xiao Shoufeng Xue Zimei Fu Man Zhao Li Zhang Junming Zhang Haishun Wu Jianfeng Jia Nianjun Yang Key Laboratory of Magnetic Molecules&Magnetic Information Materials(Ministry of Education) School of Chemistry and Materials ScienceShanxi Normal UniversityTaiyuan 030032China Department of Chemistry Hasselt University3590 DiepenbeekBelgium

Developing high-activity and low-cost catalysts is the key to eliminate the limitation of sluggish anodic oxygen evolution reaction(OER)during electrocatalytic overall water splitting.Herein,Ni‒Fe/black phosphorous(BP)composites are synthesized using a simple three-electrode system,where exfoliation of bulky BP and synthesis of NiFe composites are simultaneously achieved.Under light illumination,the optimized Ni‒Fe/BP composite exhibits excellent photoelectrocatalytic OER performance(e.g.,the overpotential is 58 mV lower than a commercial RuO_(2) electrocatalyst at a current density of 10 mA·cm^(-2)).The electron transfer on this composite is proved to follow a Ni‒BP‒Fe pathway.The electronic structure of this Ni‒Fe/BP composite is effectively regulated,leading to optimized adsorption strength of the intermediate OH*and improved intrinsic activity for the OER.Together with active sites on the support,this Ni‒Fe/BP composite possesses abundant electrochemical active sites and a bug surface area for the OER.The introduction of light further accelerates the electrocatalytic OER.This work provides a novel and facile method to synthesize high-performance metal/BP composites as well as the approaches to reveal their OER mechanisms.

关键词： black phosphorous (photo-)electrocatalysis oxygen evolution reaction

Surface facets dependent oxygen evolution reaction of single Cu_(2)O nanoparticles

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Chinese Chemical Letters 2022年第12期33卷 5158-5161页

作者： Yun Shan Xiaoli Deng Xiaoxi Lu Cong Gao Yingjian Li Qianjin Chen State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of ChemistryChemical Engineering and BiotechnologyDonghua UniversityShanghai 201620China

Understanding and establishing the structure-activity relation of nanoparticles is a prerequisite for rational design of high-performance electrocatalysts.Cu_(2)O nanoparticles enclosed with different crystal facets,namely,o-Cu_(2)O NPs with{111}facets,c-Cu_(2)O NPs with{100}facets are prepared and their electrocatalytic properties for oxygen evolution reaction(OER)in alkaline condition are evaluated at single nanoparticle level with a combination of scanning electrochemical cell microscopy and scanning electron microscopy.It is found that the o-Cu_(2)O NPs have significantly superior OER electrocatalytic activity compared to c-Cu_(2)O,which is almost inert.The estimated turnover frequency(TOF)at 1.97 V vs.RHE on{111}facet increases from 4 s^(-1) to 115 s^(-1) with the octahedron edge length decreasing from 1.3μm to 100 nm.Deposition of carbon on c-Cu_(2)O surface barely promotes the activity,suggesting the inherent poor electric conductivity within the nanocrystal is most likely the reason for low activity.This work provides direct probing to single transition metal oxide crystals with dramatically different activity.

关键词： oxygen evolution reaction Cu_(2)O nanoparticle Facets Scanning electrochemical cell microscopy Single-particle analysis

Bimetallic cobalt-nickel coordination polymer electrocatalysts for enhancing oxygen evolution reaction

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Chinese Chemical Letters 2022年第6期33卷 2928-2932页

作者： Lele Lu Qiang Li Jia Du Wei Shi Peng Cheng Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry(MOE)Renewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China

Coordination polymers(CPs)have great potential to be used in electrocatalysis owing to their designable compositions and structures.It is highly challenging to apply CPs as electrocatalysts for oxygen evolution reaction(OER)on account of insufficient catalytic efficiency and relatively poor stability of current electrocatalysts.Herein,through a mixed-metal strategy,one-dimensional Co_(x)Ni_(1-x)-HIPA with dual active sites was synthesized and studied for OER electrocatalysts.By changing the metal ratio of CoxNi1-x-HIPA,the OER performance was well regulated.The optimized Co_(1/2)Ni_(1/2)-HIPA exhibited minimum reaction activation energy,and represented an overpotential of 367 m V to reach 10 mA/cm^(2) at 25℃.Moreover,an overpotential of 314 m V at 10 m A/cm^(2) was obtained from Co_(1/2)Ni_(1/2)-HIPA at 55℃.This mixed-metal strategy provides a feasible way for adjusting the electronic states of the electrocatalysts to improve the electrocatalytic OER performance.

关键词： Coordination polymer Mixed-metal strategy Electrocatalysis oxygen evolution reaction Activation energy

Hetero MOF-on-MOF-derived carbon nanotube interconnected nitrogen-doped carbon-encapsulated FeNi/FeF2 for efficient oxygen evolution reaction

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Carbon Energy 2022年第5期4卷 924-938页

作者： Yang Zhou Hui Liu Xiaocong Gu Xiang Wu Ligang Feng School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsuPR China School of Materials Science and Engineering Shenyang University of TechnologyShenyangLiaoningPR China

Heterostructures derived from metal–organic frameworks(MOFs)with multicomponent synergism are significant in the energy conversion and catalysis reactions.Herein,we demonstrated such an efficient catalyst with the structure of self-catalyzed nitrogen-doped carbon nanotube interconnected FeNi/FeF2 derived from hetero-zeolite imidazolate frameworks 8(ZIF-8)on Fe2Ni MIL(MIL represents Materials of Institut Lavoisier)for oxygen evolution reaction.The obtained catalyst showed efficient synergism of the multicomponents,high polarity,more active sites exposure,increased intrinsic activity,and improved conductivity and stability by a carbon interconnected and confined structure as revealed by the spectroscopic analysis and electrochemical measurements.It required an overpotential of only ca.240mV(no iR correction)to reach the current density of 10mAcm^(−2) in a KOH solution when loaded on an inert glass carbon electrode,much better than similar kinds of catalysts.The improved catalytic performance can be well correlated to the structural transformation step by step from different MOFs to their derivatives by subsequent carbonation and fluorination.Because of the above-mentioned structural advantages,good catalysis performance of high activity and stability,faster catalytic kinetics,and facile active phase formation were observed compared to those of other similar materials.This work offers a new platform of derivatives from hetero MOF-on-MOF for catalysis reactions.

关键词： FeNi MOF-on-MOF,multicomponent synergism N-doped carbon nanotube oxygen evolution reaction

Acidic oxygen evolution reaction:Mechanism,catalyst classification,and enhancement strategies

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Interdisciplinary Materials 2023年第1期2卷 53-90页

作者： Qianli Ma Shichun Mu Fuel cell Materials Laboratory Foshan Xianhu LaboratoryFoshanChina State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhanChina

As the most desirable hydrogen production device,the highly efficient acidic proton exchange membrane water electrolyzers(PEMWE)are severely limited by the sluggish kinetics of oxygen evolution reaction(OER)at the anode.Rutile IrO2 is a commercial acid-stable OER catalyst with poor activity and high cost,which has motivated the development of alternatives.However,hitherto most of the designed acidic OER catalysts have disadvantages of low activity or stability,which cannot meet the requirement of industrial applications.Thus,exploring suitable strategies to enhance the activity and stability of cost-effective acidic OER catalysts is crucial for developing the PEMWE technique.In this review,the main OER mechanisms,different types of catalysts,and their activity and stability characteristics are summarized and discussed,and then possible strategies to improve activity and stability are proposed.Finally,the problems and prospects of such catalysts are generalized to shed some light on the future research of advanced catalysts for acidic OER.

关键词： catalyst hydrogen energy oxygen evolution reaction proton exchange membrane water electrolyzer water oxidation

Single-atom Fe Embedded Co_(3)S_(4) for Efficient Electrocatalytic oxygen evolution reaction

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Chemical Research in Chinese Universities 2022年第5期38卷 1282-1286页

作者： QI Yuxue LI Tingting HU Yajie XIANG Jiahong SHAO Wenqian CHEN Wenhua MU Xueqin LIU Suli CHEN Changyun YU Min MU Shichun Key Laboratory of Advanced Functional Materials of Nanjing Nanjing Xiaozhuang UniversityNanjing 211171P.R.China Co-Innovation Center of Efficient Processing and Utilization of Forest Resources College of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037P.R.China State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Wuhan University of TechnologyWuhan 430070P.R.China

Constructing atomically dispersed active sites with densely exposed and dispersed double metal-Sx catalytic sites for favorable OER catalytic activity remains rare and challenging.Herein,we design and construct a Fe_(1)S_(x)@Co_(3)S_(4) electrocatalyst with Fe single atoms epitaxially confined in Co_(3)S_(4) nanosheets for catalyzing the sluggish alkaline oxygen evolution reaction(OER).Consequently,in ultralow concentration alkaline solutions(0.1 mol/L KOH),such a catalyst is highly active and robust for OER with low overpotentials of 300 and 333 mV at current densities of 10 and 30 mA/cm^(2),respectively,accompanying long-term stability without significant degradation even for 350 h.In addition,Fe_(1)S_(x)@Co_(3)S_(4) shows a turnover frequency(TOF)value of 0.18 s−1,nearly three times that of Co_(3)S_(4)(0.07 s−1),suggesting the higher atomic utilization of Fe single atoms.Mössbauer and in-situ Raman spectra confirm that the OER activity of Fe_(1)S_(x)@Co_(3)S_(4) origins from a thin catalytic layer of Co(Fe)OOH that interacts with trace-level Fe species in the electrolyte,creating dynamically stable active sites.Combined with experimental characterizations,it suggests that the most active S-coordinated dual-metal site configurations are 2S-bridged(Fe-Co)S4,in which Co-S and Fe-S moieties are shared with two S atoms,which can strongly regulate the adsorption energy of reaction intermediates,accelerating the OER reaction kinetics.

关键词： Electrocatalyst Dual-metal site S coordination Fe single atom oxygen evolution reaction

Mitigating the Reconstruction of Metal Sulfides for Ultrastable oxygen evolution at High Current Density

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CCS Chemistry 2024年第1期6卷 137-148页

作者： Shuai Niu Tang Tang Yuanju Qu Yuyun Chen Hao Luo Hui Pan Wen-Jie Jiang Jianan Zhang Jin-Song Hu Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Nanostructure and NanotechnologyInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoMacao SAR 999078 Department of Chemical Engineering University of MelbourneParkvilleVictoria 3010 College of Materials Science and Engineering Zhengzhou UniversityZhengzhou 450001 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Dalian National Laboratory for Clean Energy Dalian 116023

Metal sulfides are emerging highly active electrocatalysts for the oxygen evolution reaction(OER),but still suffer from the instability caused by their inevitable reconstruction,especially at industrial-level current density.Here,it is discovered that Fe-incorporated Ni3S2 nanowires can deliver extraordinary durability with an ultralow potential degradation rate of 0.006 mV/h in alkaline electrolytes made with fresh water and seawater at a benchmark of 500 mA cm^(-2) while meeting the industrial activity requirement for overpotential less than 300 mV(290 mV).Systematic experiments and theoretical simulations suggest that after forming the S-doped NiFeOOH shell to boost intrinsic activity,Fe incorporation effectivelymitigates the reconstruction of the Ni_(3)S_(2) nanowire core by restraining Ni oxidation and S dissolution,justifying the performance.This work highlights the significance of circumventing reconstruction and provides a strategy to explore practical chalcogenides-based OER electrocatalysts.

关键词： oxygen evolution reaction sulfur-doped NiFeOOH NiFe sulfides nanowire ultrastable high current density

A potential-driven switch of activity promotion mode for the oxygen evolution reaction at Co_(3)O_(4)/NiO_(x)H_(y) interface

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eScience 2022年第4期2卷 438-444页

作者： Wang Wang Zixu Wang Youcheng Hu Yucheng Liu Shengli Chen Electrochemical Power Sources Key Laboratory Department of ChemistryWuhan UniversityWuhan430072China Wuhan University Testing Center Wuhan UniversityWuhan430072China

Co_(3)O_(4)spinel oxides have manifested promising activity toward the oxygen evolution reaction(OER)through effective modifications.For them to become top electrocatalysts,however,accurate accounts of the catalytic kinetics are essential to gain a deep understanding of the activity promotion mechanisms.Herein,we use a newly proposed kinetic model based on energetic span as the rate-determining term for the electrocatalytic reaction to throw light on the promotion mechanism of Co_(3)O_(4)interfaced with nickel hydroxides(NiO_(x)H_(y))for the OER.We find that depending on the electrode potential,the OER kinetics at the designed interface between Co_(3)O_(4)and NiO_(x)H_(y)are boosted in entirely different ways.As a result,the OER can occur at a lower onset potential as well as a low Tafel slope.This work emphasizes the benefit of using rational theoretical models for electrocatalyst design.

关键词： oxygen evolution reaction Interface engineering Double exchange interaction Potential-driven switch of mechanism Energetic span