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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 ***,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 *** 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 ***-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 *** functional theory(DFT)reveals that the synergy between Ni and Fe reduces the energy barrier and accelerates the rate-determining *** addition,the ultra-thin 2D sheet structure and the close combination of Ni3FeOOH and highly conductive NF support ensure the high catalytic OER ***,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

Interface engineering of Fe-Sn-Co sulfide/oxyhydroxide heterostructural electrocatalyst for synergistic water splitting

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Nano Research Energy 2024年第2期3卷 31-38页

作者： Siyu Chen Ting Zhang Jingyi Han Hui Qi Shihui Jiao Changmin Hou 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

To realize large-scale hydrogen production by electrolysis of water,it is essential to develop non-precious metal catalysts for oxygen evolution reaction(OER)and hydrogen evolution reaction(HER).Here,we fabricate Sn-,Fe-,and Co-based sulfide/oxyhydroxide heterostructural catalyst on nickel foam(FeSnCo_(0.2)S_(x)O_(y)/NF)by solvothermal *** FeSnCo_(0.2)S_(x)O_(y)/NF requires low overpotentials of 48 and 186 mV at 10 mA·cm^(-2),respectively,for HER and *** it is assembled into an electrolytic cell as a bifunctional electrocatalyst,it only needs 1.54 V to reach 10 mA·cm^(-2),far better than IrO_(2)||Pt/C *** formation of sulfide/hydroxide heterostructural interfaces improves the electron transfer and reduces the reaction energy barrier,thus promoting the electrocatalytic processes.

关键词： oxygen evolution reaction hydrogen evolution reaction overall water splitting sulfide bifunctional electrocatalyst

Multicomponent transition metal oxides and(oxy)hydroxides for oxygen evolution

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Nano Research 2023年第2期16卷 1913-1966页

作者： Jingyi Han jingqi guan Institute of Physical Chemistry College of ChemistryJilin UniversityChangchun 130021China

Oxygen evolution reaction(OER)is the core electrode reaction in energy-related technologies,such as electrolytic water,electrocatalytic carbon dioxide reduction,rechargeable metal-air batteries,and renewable fuel *** of well-stocked,cost-effective,and high-performance OER electrocatalysts is the key to the improvement of energy efficiency and the large-scale commercial implementation of these *** transition metal oxides and(oxy)hydroxides are the most promising OER catalysts due to their low cost,adjustable structure,high electrocatalytic activity,and outstanding *** this review,a brief overview about the mechanisms of OER is first offered,accompanied with the theory and calculation ***,the latest advances in the rational design of the related OER electrocatalysts and the modulation of the electronic structure of active sites are comprehensively ***,various strategies(including element doping,defect engineering,and fabrication of binderless catalysts)used to improve the OER performance are detailedly discussed,emphasizing the structure–function ***,the challenges and perspectives on this promising field are proposed.

关键词： oxyhydroxide mixed oxide oxygen evolution reaction single-atom catalyst water splitting

Applications of single-atom catalysts

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Nano Research 2022年第1期15卷 38-70页

作者： Qiaoqiao Zhang jingqi guan Institute of Physical Chemistry College of ChemistryJilin UniversityChangchun 130012China

Owing to unsaturated coordination environment,quantum size effect and metal-support interaction,single-or dual-atom metal sites,such as Mn,Fe,Co,Ni,Cu,Zn,Mo,Ru,Rh,Pd,Ag,Sn,Ir,Pt,Au,Bi,and Er coordinated with nonmetallic elements such as O,N,P,and S,exhibit different electronic configurations,which endow them with high catalytic performances in multiple redox reactions and versatile applications in organic synthesis,environmental remediation,energy conversion,and *** intense research,the relation of structure-activity for single-atom catalysts(SACs)still bedazzles researchers,since diversified configurations of active sites would bring about difficulty in structural identification and theoretical ***,recent results on the applications of SACs are reviewed with an emphasis on identifying the active sites and discussing the relation between structure and property.

关键词： biomedicine energy conversion environmental remediation organic synthesis single-atom catalysis

Self-supported transition metal chalcogenides for oxygen evolution

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Nano Research 2023年第7期16卷 8684-8711页

作者： Ting Zhang Jianrui Sun jingqi guan Institute of Physical Chemistry College of ChemistryJilin University2519 Jiefang RoadChangchun 130021China School of Chemistry and Life Science Changchun University of TechnologyChangchun 130012China

Owing to stable spatial framework and large electrochemical interface,self-supported transition metal chalcogenides have been actively explored in renewable energy fields,especially in oxygen evolution reaction(OER).Here,we review the research progress of self-supported transition metal chalcogenides(including sulfides,selenides,and tellurides)for the OER in recent *** basic principle and evaluation parameters of OER are first introduced,and then the preparation methods of transition metal chalcogenides on various self-supporting substrates(including Ni foam(NF),carbon cloth(CC),carbon fiber paper(CFP),metal mesh/plate,etc.)are systematically ***,advanced optimization strategies(including interface and defect engineering,heteroatom doping,edge engineering,surface morphology engineering,and construction of heterostructure)are introduced in detail to improve the inherent catalytic activity of self-supported ***,the challenges and prospects of developing more promising self-supported chalcogenide electrocatalysts are proposed.

关键词： self-supported chalcogenide oxygen evolution reaction(OER) interface and defect engineering heteroatom doping heterostructure

Recent progress and prospect of carbon-free single-site catalysts for the hydrogen and oxygen evolution reactions

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Nano Research 2022年第2期15卷 818-837页

作者： jingqi guan Xue Bai Tianmi Tang Institute of Physical Chemistry College of ChemistryJilin University2519 Jiefang RoadChangchun 130021China

The key challenge for scalable production of hydrogen from water lies in the rational design and preparation of high-performance and earth-abundant electrocatalysts to replace precious metal Pt and IrO_(2) for hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).Although atomic M-N-C materials have been extensively studied in heterogeneous catalysis field,the insufficient antioxidant capacity of carbonous substrates hinders their practical application in *** highly active and stable OER electrocatalysts is the key for electrochemical water *** review presents feasible design strategies for fabricating carbon-free single-site catalysts and their applications in HER/OER and overall water *** constitutive relationships between structure,composition,and catalytic performance for HER and OER are detailly discussed,providing ponderable insights into rationally constructing high-performance HER and OER *** perspectives on the challenges and future research orientations in single-site catalysts for electrochemical water splitting are suggested.

关键词： single-atom catalyst single-site catalyst hydrogen evolution reaction oxygen evolution reaction water splitting

The d-orbital regulation of isolated manganese sites for enhanced oxygen evolution

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Nano Research 2023年第8期16卷 10796-10802页

作者： Xue Bai Jingyi Han Xiaodi Niu jingqi guan Institute of Physical Chemistry College of ChemistryJilin University2519 Jiefang RoadChangchun 130021China College of Food Science and Engineering Jilin UniversityChangchun 130062China

Developing transition metal-nitrogen-carbon materials(M-N-C)as electrocatalysts for the oxygen evolution reaction(OER)is significant for low-cost energy conversion *** d-orbital adjustment of M center in M-N-C is beneficial to the improvement of OER ***,we synthesize a single-Mn-atom catalyst based on carbon skeleton(Mn_(1)-N_(2)S_(2)C_(x))with isolated Mn-N_(2)S_(2)sites,which exhibits high alkaline OER activity(η10=280 mV),low Tafel slope(44 mV·dec^(−1)),and excellent *** calculations reveal the pivotal function of isolated Mn-N_(2)S_(2)sites in promoting OER,including the adsorption kinetics of intermediates and activation mechanism of active *** doping of S causes the increase in both charge density and work function of active Mn center,and ortho-Mn_(1)-N_(2)S_(2)C_(x)expresses the fastest OER kinetics due to the asymmetric plane.

关键词： dual-heteroatom coordination Mn1-N_(2)S_(2)C_(x) oxygen evolution reaction(OER) single-atom catalyst theoretical calculation

Advances and challenges in two-dimensional materials for oxygen evolution

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Nano Research 2022年第10期15卷 8714-8750页

作者： Tianmi Tang Saisai Li Jianrui Sun Zhenlu Wang jingqi guan Institute of Physical Chemistry College of ChemistryJilin UniversityChangchun 130021China School of Chemistry and Life Science Changchun University of TechnologyChangchun 130012China

Oxygen evolution reaction(OER)plays an important role in many energy conversions and storage technologies,such as water splitting,rechargeable metal air batteries,renewable fuel cells,and electrocatalytic carbon dioxide reduction and nitrogen reduction,but its slow kinetics and high overpotential seriously affect the energy *** of high-performance and well-stocked OER catalysts is the key to the large-scale implementation of these energy-related ***-dimensional(2D)materials get a lot of attention as OER catalysts due to their large specific surface area,abundant active sites,and adjustable structures and ***,an overview is presented for the latest achievements in design and synthesis of 2D materials(including layered double hydroxides,metal-organic frameworks and their derivatives,covalent-organic frameworks,graphene,and black phosphorus)for the OER,emphasizing novel strategies(including metal/nonmetal doping,defect engineering,interface engineering,lattice strain,and fabrication of heterojunction)for achieving high electrocatalytic ***,the structure–function relationship is analyzed in detail to gain deeper insight into the reaction mechanism,which is crucial to rational design of more high-performance 2D materials for the ***,the remaining challenges to improve the OER performance of 2D electrocatalysts are put forward to indicate possible future development of 2D materials.

关键词： two-dimensional material oxygen evolution reaction layered double hydroxide metal-organic framework covalentorganic framework

Atomic manganese coordinated to nitrogen and sulfur for oxygen evolution

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Nano Research 2022年第7期15卷 6019-6025页

作者： Xue Bai Liming Wang Bing Nan Tianmi Tang Xiaodi Niu jingqi guan Institute of Physical Chemistry College of ChemistryJilin University2519 Jiefang RoadChangchun 130021China College of Food Science and Engineering Jilin UniversityChangchun 130062China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety&CAS-HKU Joint Laboratory of Metallomics on Health and Environment Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China State Key Laboratory of Natural and Biomimetic Drugs School of Pharmaceutical SciencesPeking UniversityBeijing 100191China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of ScienceShanghai 201210China

Lack of high-efficiency,cost-efficient,and well-stocked oxygen evolution reaction(OER)electrocatalysts is a main challenge in large-scale implementation of electrolytic *** regulating the electronic structure of isolated single-atom metal sites,highperformance transition-metal-based catalysts can be fabricated to greatly improve the OER ***,we demonstrate single-atom manganese coordinated to nitrogen and sulfur species in two-dimensional graphene nanosheets MnNSG(NSG means N-and S-codoped graphene)as an active and durable OER catalyst with a low overpotential of 296 mV in alkaline media,compared to that of the benchmark IrO_(2) *** calculations and experimental measurements reveal that the Mn-N3S sites in the graphene matrix are the most active sites for the OER due to modified electronic structure of the Mn site by three nitrogen and one sulfur atoms coordination,which show lower theoretical overpotential than the Mn-N4 sites and over which the O–O formation step is the rate-determining step.

关键词： Mn-N-C N/S co-coordination oxygen evolution reaction single-atom catalyst theoretical calculations