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surface reconstruction and structural transformation of twodimensional Ni-Fe MOFs for oxygen evolution in seawater media

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Nano Research 2024年第4期17卷 2429-2437页

作者： Liyuan Xiao Xue Bai Jingyi Han Tianmi Tang Siyu Chen Hui Qi Changmin Hou Fuquan Bai Zhenlu Wang Jingqi Guan Institute of Physical Chemistry College of ChemistryJilin UniversityChangchun 130021China The Second Hospital of Jilin University Changchun 130021China State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun 130012China Laboratory of Theoretical and Computational Chemistry Institute of Theoretical ChemistryCollege of ChemistryChangchun 130023China

As a four-electron transfer reaction,oxygen evolution reaction(OER)is limited by large overpotential and slow kinetics.Here,we in-situ synthesized two-dimensional(2D)Ni-Fe metal-organic framework nanosheets on nickel foam(NixFe-TPA/NF,TPA=terephthalic acid)for oxygen evolution in alkaline and alkaline seawater electrolytes.In 1 M KOH,Ni3Fe-TPA/NF shows a low overpotential(η10)of 189 mV at 10 mA·cm^(-2) and an ultra-low overpotential of only 260 mV at 500 mA·cm^(-2).In alkaline seawater,Ni3Fe-TPA/NF still provides impressive OER performance,with anη10 of 265 mV.In-situ Raman characterization results show that the phase transition occurs during the OER,and Ni3FeOOH with more oxygen vacancies is in-situ formed,reducing the OER energy barrier.Density functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining step.In addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER activity.Therefore,the surface reconstruction and structural modification strategy can be used to design and prepare high-performance OER electrocatalysts for energy-related applications.

关键词： density functional theory(DFT)calculation Ni3FeOOH oxygen evolution reaction seawater electrolysis surface reconstruction

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surface reconstruction of heterostructures in alkaline medium towards enhanced electrocatalytic hydrogen evolution

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Rare Metals 2024年第6期43卷 2636-2647页

作者： Ming-Yang Yang Ji Yuan Xue-Lian Fu Jing-Jing Chen Jing Hu Zhou-Guang Lu Chen Liu Guangdong Research Center for Interfacial Engineering of Functional Materials Shenzhen Key Laboratory of Polymer Science and TechnologyShenzhen Key Laboratory of Energy Electrocatalytic MaterialsCollege of Materials Science and EngineeringShenzhen University Shenzhen Key Laboratory of Interfacial Science and Engineering of Materials Department of Materials Science and EngineeringSouthern University of Science and Technology

Constructing heterostructures has proved to be a successful strategy to fabricate electrocatalysts with high efficiency for water splitting.However,the structure evolution in alkaline hydrogen evolution reaction lacks investigation and the specific active center remains disputable.Herein,we take the well-designed Ni3S2@VO2heterostructures as a model to investigate the electrocatalytic activity and the surface reconstruction process of heterostructure catalysts in alkaline electrolyte.The Ni3S2@VO2heterostructures,with Ni3S2nanorods as the core and VO2nanoflakes as the shell,coupled with the high conductive Ni3S2,the hydrophilic VO2and modulated electronic structures at the interfaces,exhibited prominent activity and superior stability at various current densities.Further,the ex-situ characterizations confirmed that the surface reconstruction from Ni3S2@VO2into Ni3S2@amorphous-Ni（OH）2in alkaline media could optimize the water dissociation barrier and exposed large active area,thereby contributing to improved electrocatalytic performance.Our study not only introduces novel high-performance electrocatalysts for hydrogen evolution reaction（HER）,but also provides a new avenue for re-examining hetero-structural catalysts in alkaline solutions.

关键词： Heterostructures Ni 3 S 2 @VO 2 surface reconstruction Water dissociation Alkaline hydrogen evolution

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Covalency competition induced selective bond breakage and surface reconstruction in manganese cobaltite towards enhanced electrochemical charge storage

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Green Energy & Environment 2024年第5期9卷 909-918页

作者： Peng Gao Pei Tang Ying Mo Peitao Xiao Wang Zhou Shi Chen Hongliang Dong Ziwei Li Chaohe Xu Jilei Liu College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangshaHunan410082China Department of Materials Science and Engineering National University of Defense TechnologyChangshaHunan410073China Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoAvenida da UniversidadeTaipaMacao999078China Center for High Pressure Science and Technology Advanced Research PudongShanghai201203China College of Aerospace Engineering Chongqing UniversityChongqing400044China

Manganese cobaltite(MnCo_(2)_(4))is a promising electrode material because of its attractive redox chemistry and excellent charge storage capability.Our previous work demonstrated that the octahedrally-coordinated Mn are prone to react with the hydroxyl ions in alkaline electrolyte upon electrochemical cycling and separates on the surface of spinel to reconstruct into d-MnO_(2) nanosheets irreversibly,thus results in a change of the reaction mechanism with Kþion intercalation.However,the low capacity has greatly limited its practical application.Herein,we found that the tetrahedrally-coordinated Co_(2) þions were leached when MnCo_(2)_(4) was equilibrated in 1 mol L^(-1) HCl solution,leading to the formation of layered CoOOH on MnCo_(2)_(4) surface which is originated from the covalency competition induced selective breakage of the CoT–O bond in CoT–O–CoO and subsequent rearrangement of free Co_(6) octahedra.The as-formed CoOOH is stable upon cycling in alkaline electrolyte,exhibits conversion reaction mechanism with facile proton diffusion and is free of massive structural evolution,thus enables utilization of the bulk electrode material and realizes enhanced speciﬁc capacity as well as facilitated charge transfer and ion diffusion.In general,our work not only offers a feasible approach to deliberate modiﬁcation of MnCo_(2)_(4)'s surface structure,but also provides an in-depth understanding of its charge storage mechanism,which enables rational design of the spinel oxides with promising charge storage properties.

关键词： Manganese cobaltite Tetrahedrally-coordinated Co^(2+)leaching Selective bond breakage surface reconstruction Charge storage mechanisms

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Steering surface reconstruction of hybrid metal oxides for efficient oxygen evolution reaction in water splitting and zinc-air batteries

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Journal of Energy Chemistry 2024年第5期92卷 383-393页

作者： Jie Zhu Junxue Chen Xida Li Kun Luo Zewei Xiong Zhiyu Zhou Wenyun Zhu Zhihong Luo Jingbin Huang Yibing Li Key Lab of New Processing Technology for Nonferrous Metals and Materials Ministry of EducationSchool of Materials Science and EngineeringGuilin University of TechnologyGuilin 541000GuangxiChina The Key Laboratory of Rare Earth Functional Materials and Applications Zhoukou Normal UniversityZhoukou 466001HenanChina School of Chemistry and Chemical Engineering Beijing Institute of TechnologyBeijing 100081China School of Materials Science and Engineering Changzhou UniversityChangzhou 213164JiangsuChina Wuhan Sunmoon Battery Co. LtdWuhan 430090HubeiChina

surface reconstruction yields real active species in electrochemical oxygen evolution reaction(OER)conditions;however,rationally regulating reconstruction in a targeted manner for constructing highly active OER electrocatalysts remains a formidable challenge.Here,an electrochemical activation strategy with selective etching was utilized to guide the reconstruction process of a hybrid cobalt-molybdenum oxide(CoMoO_(4)/Co_(3)O_(4)@CC)in a favorable direction to improve the OER performance.Both in-situ Raman and multiple ex-situ characterization tools demonstrate that controlled surface reconstruction can be easily achieved through Mo etching,with the formation of a dynamically stable amorphous-crystalline heterostructure.Theoretical calculations together with experimental results reveal that the synergistic effects between amorphous CoOOH and crystalline Co_(3)O_(4) are crucial in enhancing the catalytic performance.Consequently,the reconstructed CoMoO_(4)/Co_(3)O_(4)@CC exhibits a low overpotential of 250 mV to achieve a current density of 10 mA cm^(-2) in 1 M KOH,and more importantly it can be practiced in electrolytic water splitting and rechargeable zinc-air batteries devices,achieving ultra-long stability for over 500 and 1200 h,respectively.This work provides a promising route for the construction of high-performance electrocatalysts.

关键词： Electrocatalyst Oxygen evolution reaction surface reconstruction Selective etching Amorphous-crystalline heterostructures

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Controllable surface reconstruction of copper foam for electrooxidation of benzyl alcohol integrated with pure hydrogen production

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SmartMat 2024年第1期5卷 147-157页

作者： Yingnan Han Chang Yu Hongling Huang Qianbing Wei Junting Dong Lin Chen Jieshan Qiu State Key Lab of Fine Chemicals School of Chemical EngineeringLiaoning Key Lab for Energy Materials and Chemical EngineeringDalian University of TechnologyDalianChina State Key Laboratory of Chemical Resource Engineering College of Chemical EngineeringBeijing University of Chemical TechnologyBeijingChina

Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine chemicals.Herein,we focus on an electrochemical redox activation strategy to rationally manipulate the microstructure and surface valence states of copper foam(CF)and boost the corresponding performance towards electrocatalytic benzyl alcohol oxidation(EBA),accompanied by the efficient hydrogen production.Correspondingly,the Cu(II)‐dominated species are gradually formed on the CF surface with the dissolution and redeposition of copper in the suitable potential range.The new species containing Cu2O,CuO,and Cu(OH)2 during surface reconstruction process of the CF were confirmed by multiple characterization techniques.After 220‐cycled activation(CF‐220),the activated CF achieves an increase of current density for EBA in anode from 9.5 for the original CF to 29.3 mmol/cm2,while the pure hydrogen yield increases threefold than that of the original CF at 1.5 VRHE.The produced new species can endow the CF‐220 with abundant acidity sites,which can enhance the adsorption toward Lewis‐basicity benzyl alcohol,confirmed by NH3‐temperature‐programmed desorption.In situ Raman result further reveals that the as‐produced CuO,Cu(OH)2,and Cu(OH)42−are the main active species toward the EBA process.

关键词： benzyl alcohol copper electrochemical oxidation Lewis acid surface reconstruction

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surface reconstruction,doping and vacancy engineering to improve the overall water splitting of CoP nanoarrays

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Nano Research 2023年第1期16卷 228-238页

作者： Yongkai Sun Wenyuan Sun Lihong Chen Alan Meng Guicun Li Lei Wang Jianfeng Huang Aili Song Zhenhui Zhang Zhenjiang Li College of Electromechanical Engineering Qingdao University of Science and TechnologyQingdao 266061China College of Materials Science and Engineering Qingdao University of Science and TechnologyQingdao 266042China Key Laboratory of Optic-electric Sensing and Analytical Chemistry for Life Science MOE College of Chemistry and Molecular EngineeringQingdao University of Science and TechnologyQingdao 266042China School of Material Science and Engineering International S&T Cooperation Foundation of Shaanxi ProvinceXi’an Key Laboratory of Green Manufacture of Ceramic MaterialsShaanxi University of Science and TechnologyXi’an 710021China Qingdao Huanghai University Qingdao 266000China

Development of a general regulatory strategy for efficient overall water splitting remains a challenging task.Herein,a simple,costfairness,and general fluorination strategy is developed to realize surface reconstruction,heteroatom doping,and vacancies engineering over cobalt phosphide(CoP)for acquiring high-performance bifunctional electrocatalysts.Specifically,the surface of CoP nanoarrays(NAs)becomes rougher,meanwhile F doped into CoP lattice and creating amounts of P vacancies by fluorination,which caused the increase of active sites and regulation of charge distribution,resulting the excellent electrocatalyst performance of F-CoP NAs/copper foam(CF).The optimized F-CoP NAs/CF delivers a lower overpotential of only 35 mV at 10 mA·cm^(−2)for hydrogen evolution reaction(HER)and 231 mV at 50 mA·cm^(−2)for oxygen evolution reaction(OER),and the corresponding overall water splitting requires only 1.48 V cell voltage at 10 mA·cm^(−2),which are superior to the most state-of-theart reported electrocatalysts.This work provides an innovative and feasible strategy to construct efficient electrocatalysts.

关键词： fluorination surface reconstruction F atom doping P vacancies overall water splitting

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surface reconstruction establishing Mott-Schottky heterojunction and built-in space-charging effect accelerating oxygen evolution reaction

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Nano Research 2022年第4期15卷 2952-2960页

作者： Yao Kang Shuo Wang Kwan San Hui Shuxing Wu Duc Anh Dinh Xi Fan Feng Bin Fuming Chen Jianxin Geng Weng-Chon(Max)Cheong Kwun Nam Hui Joint Key Laboratory of the Ministry of Education Institute of Applied Physics and Materials EngineeringUniversity of MacaoTaipaMacao 999078China Engineering Faculty of ScienceUniversity of East AngliaNorwich NR47TJUK School of Chemical Engineering and Light Industry Guangdong University of TechnologyGuangzhou 510006China NTT hi-tech institute Nguyen Tat Thanh universityHo Chi Minh city 700000Vietnam Ningbo Institute of Materials Technology EngineeringChinese Academy of SciencesNingbo 315201China State Key Laboratory of High-Temperature Gas Dynamics Institute of MechanicsChinese Academy of ScienceBeijing 100190China State Key Laboratory of Optic Information Physics and Technologies School of Physics and Telecommunication EngineeringSouth China Normal UniversityGuangzhou 510006China State Key Laboratory of Organic-Inorganic Composites Beijing University of Chemical Technology15 North Third Ring East RoadChaoyang DistrictBeijing 100029China Department of Physics and Chemistry Faculty of Science and TechnologyUniversity of MacaoTaipaMacao 999078China

Structural reconstruction of nanomaterials offers a fantastic way to regulate the electronic structure of active sites and promote their catalytic activities.However,how to properly facilitate surface reconstruction to overcome large overpotential that stimulate the surface reconstruction has remained elusive.Herein,we adopt a facile approach to activate surface reconstruction on Ni(OH)_(2) by incorporating F anions to achieve electro-derived structural oxidation process and further boost its oxygen evolution reaction(OER)activity.Ex situ Raman and X-ray photoemission spectroscopy studies indicate that F ions incorporation facilitated surface reconstruction and promotes the original Ni(OH)_(2)transformed into a mesoporous and amorphous F-NiOOH layer during the electrochemical process.Density functional theory(DFT)calculation reveals that this self-reconstructed NiOOH induces a space-charge effect on the p-n junction interface,which not only promotes the absorption of intermediates species(^(*)OH,^(*)O,and^(*)OOH)and charge-transfer process during catalysis,but also leads to a strong interaction of the p-n junction interface to stabilize the materials.This work opens up a new possibility to regulate the electronic structure of active sites and promote their catalytic activities.

关键词： F anions dynamic migration nickel hydroxides surface reconstruction oxygen evolution reaction(OER)

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surface reconstruction of Se-doped NiS_(2) enables high-efficiency oxygen evolution reaction

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Journal of Energy Chemistry 2023年第9期84卷 173-180页

作者： Mengxin Chen Yuanyuan Zhang Ran Wang Bin Zhang Bo Song Yanchao Guan Siwei Li Ping Xu MIIT Key Laboratory of Critical Materials Technology for New Energy Conversion and Storage School of Chemistry and Chemical EngineeringHarbin Institute of TechnologyHarbin 150001HeilongjiangChina National Key Laboratory of Science and Technology on Advanced Composites in Special Environments Harbin Institute of TechnologyHarbin 150001HeilongjiangChina Key Laboratory of Micro-systems and Micro-structures Manufacturing Ministry of EducationHarbin Institute of TechnologyHarbin 150001HeilongjiangChina Institute of Industrial Catalysis School of Chemical Engineering and TechnologyXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

surface reconstruction of electrocatalysts has been widely witnessed during the electrochemical processes.Here,NiS_(2),NiSe_(2), and Se doped NiS_(2)(Se-NiS_(2)) are fabricated for oxygen evolution reaction(OER) through a mild sulfuration and/or selenylation process of Ni(OH)_(2) supported on carbon cloth(CC).Through careful in-situ Raman spectroscopy and ex-situ X-ray photoelectron spectroscopy,surface reconstruction of NiS_(2),NiSe_(2),and Se-NiS_(2) during the OER process has been revealed.A potentialdependent study shows that Se-NiS_(2) undergoes surface evolution at lower potentials and requires the lowest potential for conversion to NiOOH as a highly OER-active species,accompanied by the leaching of SO_(4)^(2-) and SeO_(4)^(2-) that can again be adsorbed on the catalyst surface to enhance the catalytic activity.Density functional theory(DFT) calculations confirm that Se-NiS_(2) is more susceptible to surface oxidation through the OER process.Therefore,Se-NiS_(2) exhibits outstanding OER activity and stability in alkaline conditions,requiring an overpotential of 343 mV at a current density of 50 mA cm^(-2).A novel insight is provided by our work in understanding the surface reconstruction and electrocatalytic mechanism of Ni-based chalcogenides.

关键词： Oxygen evolution reaction Se-NiS_(2) In-situ Raman spectroscopy Anion leaching surface reconstruction

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Etching‑Induced surface reconstruction of NiMoO_(4) for Oxygen Evolution Reaction

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Nano-Micro Letters 2023年第2期15卷 271-282页

作者： Jinli Zhu Jinmei Qian Xuebing Peng Baori Xia Daqiang Gao Key Laboratory for Magnetism and Magnetic Materials of MOE Key Laboratory of Special Function Materials and Structure Design of MOELanzhou UniversityLanzhou 730000People’s Republic of China

Rational reconstruction of oxygen evolution reaction(OER)precatalysts and performance index of OER catalysts are crucial but still challenging for universal water electrolysis.Herein,we develop a double-cation etching strategy to tailor the electronic structure of NiMoO_(4),where the prepared NiMoO_(4) nanorods etched by H_(2)O_(2) reconstruct their surface with abundant cation deficiencies and lattice distortion.Calculation results reveal that the double cation deficiencies can make the upshift of d-band center for Ni atoms and the active sites with better oxygen adsorption capacity.As a result,the optimized sample(NMO-30M)possesses an overpotential of 260 mV at 10 mA cm−2 and excellent long-term durability of 162 h.Importantly,in situ Raman test reveals the rapid formation of high-oxidation-state transition metal hydroxide species,which can further help to improve the catalytic activity of NiMoO_(4) in OER.This work highlights the influence of surface remodification and shed some light on activating catalysts.

关键词： Etching surface reconstruction Cation deficiencies OER

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Cu_(2−x)S derived copper nanoparticles:A platform for unraveling the role of surface reconstruction in efficient electrocatalytic CO_(2)-to-C_(2)H_(4)conversion

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Nano Research 2023年第4期16卷 4494-4498页

作者： Chaohua He Delong Duan Jingxiang Low Yu Bai Yawen Jiang Xinyu Wang Shuangming Chen Ran Long Li Song Yujie Xiong Hefei National Laboratory for Physical Sciences at the Microscale Frontiers Science Center for Planetary Exploration and Emerging TechnologiesSchool of Chemistry and Materials Scienceand National Synchrotron Radiation LaboratoryUniversity of Science and Technology of ChinaHefei 230026China Hefei Comprehensive National Science Center 350 Shushanhu Rd.Hefei 230031China

Cu-based electrocatalysts have provoked much attention for their high activity and selectivity in carbon dioxide(CO_(2))conversion into multi-carbon hydrocarbons.However,during the electrochemical reaction,Cu catalysts inevitably undergo surface reconstruction whose impact on CO_(2)conversion performance remains contentious.Here we report that polycrystalline Cu nanoparticles(denoted as Cu-s)with rich high-index facets,derived from Cu_(2−x)S through desulphurization and surface reconstruction,offer an excellent platform for investigating the role of surface reconstruction in electrocatalytic CO_(2)conversion.During the formation of Cu-s catalyst,the two stages of desulphurization and surface reconstruction can be clearly resolved by in situ X-ray absorption spectroscopy and OH−adsorption characterizations,which are well correlated with the changes in electrocatalytic performance.It turns out that the high CO_(2)conversion performance,achieved by the Cu-s catalyst(Faradic efficiency of 68.6%and partial current density of 40.8 mA/cm^(2)in H-cell toward C_(2)H_(4)production),is attributed to the increased percentage of high-index facets in Cu-s during the surface reconstruction.Furthermore,the operando electrochemical Raman spectroscopy further reveals that the conversion of the CO_(2)into the C_(2)H_(4)on Cu-s is intermediated by the production of*COCHO.Our findings manifest that the surface reconstruction is an effective method for tuning the reaction intermediate of the CO_(2)conversion toward high-value multicarbon(C2+)chemicals,and highlight the significance of in situ characterizations in enhancing the understanding of the surface structure and its role in electrocatalysis.

关键词： CO_(2)electroreduction reaction surface reconstruction high-index facets ethylene(C_(2)H_(4)) Cu catalysts

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