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Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation

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Nano-Micro Letters 2024年第4期16卷 415-431页

作者： Qianqian Zhao Bin Zhao Xin Long Renfei Feng Mohsen Shakouri Alisa Paterson Qunfeng Xiao Yu Zhang xian‑zhu fu Jing‑Li Luo Shenzhen Key Laboratory of Energy Electrocatalytic Materials Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Canadian Light Source Inc. SaskatoonSK S7N 0X4Canada Instrumental Analysis Center of Shenzhen University(Lihu Campus) Shenzhen UniversityShenzhen 518055People’s Republic of China

Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.

关键词： Dual-monodispersed heterostructure Electronic interactive modulation Reaction mechanism Methanol oxidation reaction Hydrogen generation

Metal-organic framework-based single-atom electro-/ photocatalysts: Synthesis, energy applications, and opportunities

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Carbon Energy 2024年第1期6卷 1-43页

作者： Munir Ahmad Jiahui Chen Jianwen Liu Yan Zhang Zhongxin Song Shahzad Afzal Waseem Raza Liaqat Zeb Andleeb Mehmood Arshad Hussain Jiujun Zhang xian-zhu fu Jing-Li Luo Shenzhen Key Laboratory of Energy Electrocatalytic Materials Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhenGuangdongChina College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhenGuangdongChina College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhenGuangdongChina Department of Environmental Engineering China Jiliang UniversityHangzhouZhejiangChina Institute for Advanced Study Shenzhen UniversityShenzhenGuangdongChina School of Bioengineering Dalian University of TechnologyDalianLiaoningChina College of Materials Science and Engineering Fuzhou UniversityFuzhouFujianChina Institute for Sustainable Energy Shanghai UniversityShanghaiChina

Single-atom catalysts(SACs)have gained substantial attention because of their exceptional catalytic ***,the high surface energy limits their synthesis,thus creating significant challenges for further *** the last few years,metal–organic frameworks(MOFs)have received significant consideration as ideal candidates for synthesizing SACs due to their tailorable chemistry,tunable morphologies,high porosity,and chemical/thermal *** this perspective,this review thoroughly summarizes the previously reported methods and possible future approaches for constructing MOF-based(MOF-derived-supported and MOF-supported)***,MOF-based SAC's identification techniques are briefly assessed to understand their coordination environments,local electronic structures,spatial distributions,and catalytic/electrochemical reaction *** review systematically highlights several photocatalytic and electrocatalytic applications of MOF-based SACs for energy conversion and storage,including hydrogen evolution reactions,oxygen evolution reactions,O_(2)/CO_(2)/N_(2) reduction reactions,fuel cells,and rechargeable *** light is also shed on the future development of this highly exciting field by highlighting the advantages and limitations of MOF-based SACs.

关键词： carbon energy generation MOF-derived-supported MOF-supported single atoms

Etching oxide overlayers of NiFe phosphide to facilitate surface reconstruction for oxygen evolution reaction

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Green Energy & Environment 2022年第3期7卷 365-371页

作者： Tehua Wang xian-zhu fu Shuangyin Wang College of Materials Science and Engineering Shenzhen UniversityShenzhen518055China College of Physics and Optoelectronic Engineering Shenzhen UniversityShenzhen518060China State Key Laboratory of Chem/Bio-sensing and Chemometrics College of Chemistry and Chemical EngineeringHunan UniversityChangsha410082China

Transition-metal phosphides have been of concern as efficient electrocatalysts for oxygen evolution reaction(OER)due to its high conductivity and earth-abundance ***,oxide overlayers formed on their surface by spontaneously atmospheric oxidation are usually neglected,thus confusing the establishment of structure–performance ***,we successfully etched the oxide overlayers of NiFe phosphide(NiFeP)by a dielectric barrier discharge(DBD)plasma technique,aiming to reveal the influence of the oxide overlayers on its electrocatalytic performance for *** is found that etching the oxide overlayers can accelerate the surface reconstruction process of NiFeP and facilitate the formation of metal hydroxides,which are key intermediate phases for ***,the etched NiFeP-DBD material shows remarkably enhanced OER activity with an overpotential of 265 mV at a current density of 10 mA cm^(-2).The finding of this work probably brings a significant impact to understand the structure–performance relationship of metal phosphide in electrooxidation reaction.

关键词： surface oxide evolution

Strengthening absorption ability of Co-N-C as efficient bifunctional oxygen catalyst by modulating the d band center using MoC

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Green Energy & Environment 2023年第2期8卷 459-469页

作者： Jianwen Liu Ying Guo xian-zhu fu Jing-Li Luo Chunyi Zhi Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen University518060China Department of Materials Science and Engineering City University of Hong Kong83 Tat Chee AvenueKowloon TongHong KongChina Department of Chemical and Materials Engineering University of AlbertaEdmontonAlbertaT6G 1H9Canada

Co-N-C is a promising oxygen electrochemical catalyst due to its high stability and good ***,due to the limited adsorption ability improvement for oxygen-containing intermediates,it usually exhibits inadequate catalytic activity with 2-electron pathway and high selectivity of hydrogen ***,the adsorption of Co-N-C to these intermediates is modulated by constructing heterostructures using transition metals and their derivatives based on d-band *** heterostructured nanobelts with MoC core and pomegranate-like carbon shell consisting of Co nanoparticles and N dopant(MoC/Co-N-C)are engineered to successfully modulate the d band center of active Co-N-C sites,resulting in a remarkably enhanced electrocatalysis *** optimally performing MoC/Co-N-C exhibits outstanding bi-catalytic activity and stability for the oxygen electrochemistry,featuring a high wave-half potential of 0.865 V for the oxygen reduction reaction(ORR)and low overpotential of 370 mV for the oxygen evolution reaction(OER)at 10 mA cm^(-2).The zinc air batteries with the MoC/Co-N-C catalyst demonstrate a large power density of 180 mW cm^(-2)and a long cycling lifespan(2000 cycles).The density functional theory calculations with Hubbard correction(DFT+U)reveal the electron transferring from Co to Mo atoms that effectively modulate the d band center of the active Co sites and achieve optimum adsorption ability with"single site double adsorption"mode.

关键词： Bifunctional oxygen catalysts Pomegranate-like shell D band theory Enhanced synergistic effect Rechargeable zinc air battery

Mesoporous CeO_(2)-C hybrid spheres as efficient support for platinum nanoparticles towards methanol electrocatalytic oxidation

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Journal of Rare Earths 2021年第6期39卷 674-681,I0003页

作者： Weili Li Qi Wang Lei Wang xian-zhu fu Jing-Li Luo College of Materials Science and Engineering Shenzhen UniversityShenzhen 518060China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China Department of Chemical and Materials Engineering University of AlbertaEdmontonAlbenaT6G 2G6Canada

The development of direct methanol fuel cells(DMFCs) is partially limited by the poor kinetics of methanol oxidation reaction(MOR) at the anode *** was reported that the interaction between Pt and CeO_(2) enhances the electrocatalytic performance of Pt catalyst for *** this work,a hybrid material(CeO_(2)-C) composed of CeO_(2) and carbon was successfully prepared by a simple hydrothermal method followed by calcination in inert *** hierarchically porous nanostructure and especially good electronic conductivity of CeO_(2)-C make it an excellent support for Pt particles for application in electrocatalytic *** investigation reveals that triple-phase interface of Pt,carbon and CeO_(2) forms in Pt/CeO_(2)-C *** of the as-prepared catalyst for MOR was studied in alkaline *** Pt/CeO_(2)-C catalyst shows superior catalytic performance for MOR compared with Pt/CeO_(2) and the physical mixture of Pt/CeO_(2) and acetylene black(Pt/CeO_(2)+C).The significantly improved performance can be attributed to the synergetic effect between Pt particles and CeO_(2)-C support,and the better conductivity of CeO_(2)-*** study provides a possible method to expand the application potential of CeO_(2) materials in MOR,and may also be used in other electrocatalytic process.

关键词： Pt based catalyst Mesoporous CeO_(2)-C spheres Metal-support interaction Methanol oxidation Rare earths

A facile approach to fabricating graphene/waterborne epoxy coatings with dual functionalities of barrier and corrosion inhibitor

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Journal of Materials Science & Technology 2022年第17期112卷 263-276页

作者： Suyun Liu Xuewan Wang Qi Yin Xiongzhi xiang xian-zhu fu xian-Zong Wang Jing-Li Luo Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China State Key Laboratory of Solidification Processing Center of Advanced Lubrication and Seal MaterialsNorthwestern Polytechnical UniversityXi’an 710072China

A facile and environmentally-friendly method is developed to prepare graphene/waterborne epoxy(WEP)composite *** graphene nanosheets are produced with electrochemical-exfoliation in the solution containing surfactants,cetyl trimethyl ammonium bromide(CTAB)and sodium dodecyl sulfate(SDS).The nanosheets containing solution thus formed are subjected to a quick dialysis and then directly used as a diluent for WEP without any further *** preparation method overcomes the commonly identified problems of aggregations and‘corrosion promotion’effect associated with graphene,and increases the impedance of the composite coatings by more than two orders of *** analysis of anticorrosion performance suggested that the presence of surfactants not only improves the dispersibility of graphene nanosheets but also endows the composite coatings with both barrier and corrosion inhibition *** strategy reported herein may pave the path to the large-scale production of graphene anticorrosion coatings.

关键词： Electrochemical-exfoliation graphene Waterborne epoxy coatings Anticorrosion Inhibition

Highly selective conversion of methane to ethanol over CuFe_(2)O_(4)-carbon nanotube catalysts at low temperature

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Chinese Chemical Letters 2022年第1期33卷 390-393页

作者： Xinquan Shen Dan Wu xian-zhu fu Jing-Li Luo Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science EngineeringShenzhen UniversityShenzhen 518071China Key Laboratory of Optoelectronic Devices and Systems of Ministry of Education and Guangdong Province College of Optoelectronic EngineeringShenzhen UniversityShenzhen 518060China

Conversion of methane into liquid alcohol such as ethanol at low temperature in a straight,selective and low energy consumption process remains a topic of intense scientific research but a great *** this work,CuFe_(2)O_(4)/CNT composite is successfully synthesized via a facile co-reduction method and used as catalysts to selectively oxidize *** a low temperature of 150℃,methane is directly converted to ethanol in a single process on the as-prepared CuFe_(2)O_(4)/CNT composite with high selectivity.A mechanism is also proposed for the significant methane selective oxidation performance of the CuFe_(2)O_(4)/CNT composite catalysts.

关键词： Methane Ethanol High selectivity Synergistic effect Catalysis

Folic Acid Self-Assembly Enabling Manganese Single-Atom Electrocatalyst for Selective Nitrogen Reduction to Ammonia

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Nano-Micro Letters 2021年第8期13卷 163-174页

作者： Xuewan Wang Dan Wu Suyun Liu Jiujun Zhang xian-zhu fu Jing-Li Luo Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Institute for Sustainable Energy College of SciencesShanghai UniversityShanghai 200444People’s Republic of China

Efficient and robust single-atom catalysts(SACs)based on cheap and earth-abundant elements are highly desirable for electrochemical reduction of nitrogen to ammonia(NRR)under ambient ***,for the first time,a Mn-N-C SAC consisting of isolated manganese atomic sites on ultrathin carbon nanosheets is developed via a template-free folic acid self-assembly *** spontaneous molecular partial dissociation enables a facile fabrication process without being plagued by metal atom *** to well-exposed atomic Mn active sites anchored on two-dimensional conductive carbon matrix,the catalyst exhibits excellent activity for NRR with high activity and selectivity,achieving a high Faradaic efficiency of 32.02%for ammonia synthesis at−0.45 V versus reversible hydrogen *** functional theory calculations unveil the crucial role of atomic Mn sites in promoting N_(2) adsorption,activation and selective reduction to NH_(3) by the distal *** work provides a simple synthesis process for Mn-N-C SAC and a good platform for understanding the structure-activity relationship of atomic Mn sites.

关键词： Folic acid self-assembly N-doped carbon sheet Manganese single-atom catalyst Electrocatalysis Nitrogen reduction

Densely packed ultrafine SnO_(2) nanoparticles grown on carbon cloth for selective CO_(2) reduction to formate

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Journal of Energy Chemistry 2022年第8期31卷 159-166,I0005页

作者： Xuewan Wang Dan Wu Xiaomin Kang Jiujun Zhang xian-zhu fu Jing-Li Luo Shenzhen Key Laboratory of Polymer Science and Technology Guangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060GuangdongChina School of Materials Science and Engineering Wuhan Institute of TechnologyWuhan 430205HubeiChina Institute for Sustainable Energy College of SciencesShanghai UniversityShanghai 200444China

Electrochemical reduction of CO_(2) to fuels and chemicals is a viable strategy for CO_(2) utilization and renewable energy *** free-standing electrodes from robust and scalable electrocatalysts becomes highly ***,dense SnO_(2) nanoparticles are uniformly grown on three-dimensional(3D)fiber network of carbon cloth(CC)by a facile dip-coating and calcination ***,Zn modification strategy is employed to restrain the growth of long-range order of SnO_(2) lattices and to produce rich grain *** hybrid architecture can act as a flexible electrode for CO_(2)-to-formate conversion,which delivers a high partial current of 18.8 m A cm-2 with a formate selectivity of 80%at a moderate cathodic potential of-0.947 V *** electrode exhibits remarkable stability over a 16 h continuous *** superior performance is attributed to the synergistic effect of ultrafine SnO_(2) nanoparticles with abundant active sites and 3D fiber network of the electrode for efficient mass transport and electron *** sizeable electrodes hold promise for industrial applications.

关键词： Densely packed SnO_(2)nanoparticles Grain boundary Defect site Flexible electrode Electrochemical reduction CO_(2)to formate conversion