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Reversed charge transfer induced by nickel in Fe-Ni/Mo_(2)C@nitrogen-doped carbon nanobox for promoted reversible oxygen electrocatalysis

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Journal of Energy Chemistry 2024年第1期88卷 202-212,I0005页

作者： Zhicheng Nie Lei Zhang Qiliang Zhu Zhifan Ke yingtang zhou Thomas Wågberg Guangzhi Hu School of Materials Science and Engineering Anhui University of Science and TechnologyHuainan 232001AnhuiChina Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental ScienceYunnan UniversityKunming 650504YunnanChina National Engineering Research Center for Marine Aquaculture Marine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004ZhejiangChina Department of Physics UmeåUniversityUmeåS-90187Sweden

The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption energies of reaction intermediates,and ultimately impacts the catalytic performance.In this study,we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid system.Specifically,electrons were transferred from the metal-based species to N-doped carbon,while the carbon support reciprocally donated electrons to the metal domain upon the introduction of nickel.This led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo_(2)C@nitrogen-doped carbon catalyst,with a half-wave potential of 0.91 V towards oxygen reduction reaction(ORR)and a low overpotential of 290 m V at 10 mA cm^(-2)towards oxygen evolution reaction(OER)under alkaline conditions.Additionally,the Fe-Ni/Mo_(2)C@carbon heterojunction catalyst demonstrated high specific capacity(794 mA h g_(Zn)~(-1))and excellent cycling stability(200 h)in a Zn-air battery.Theoretical calculations revealed that Mo_(2)C effectively inhibited charge transfer from Fe to the support,while secondary doping of Ni induced a charge transfer reversal,resulting in electron accumulation in the Fe-Ni alloy region.This local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process,enhancing the catalytic efficiency of both ORR and OER.Consequently,our findings underscore the potential of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.

关键词： Metal-support interaction Charge transfer reversal Oxygen reduction reaction Oxygen evolution reaction Zinc-air battery

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Construction of ZnO@CDs@Co_(3)O_(4) sandwich heterostructure with multi-interfacial electron-transfer toward enhanced photocatalytic CO_(2) reduction

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Chinese Chemical Letters 2024年第4期35卷 147-152页

作者： Xiuzheng Deng Yi Ke Jiawen Ding yingtang zhou Hui Huang Qian Liang Zhenhui Kang Advanced Catalysis and Green Manufacturing Collaborative Innovation Center CNPC-CZU Innovation AllianceSchool of Petrochemical EngineeringChangzhou UniversityChangzhou 213164China Institute of Functional Nano&Soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesSoochow UniversitySuzhou 215123China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004China

Photocatalytic conversion of CO_(2) into small-molecule chemical feedstocks can meet the growing demand for energy and alleviate the global warming. Herein, a p-n ZnO@CDs@Co_(3)O_(4) heterojunction with sandwich structure was constructed by calcination method of self-assembled ZIF-8@CDs@ZIF-67. The ZnO@CDs@Co_(3)O_(4) with well-defined interfacial structure exhibited the significantly enhanced photocatalytic CO_(2) reduction activity, and the optimal catalyst indicated the(CO + CH_(4)) evolution rate of 214.53μmol g^(-1)h^(-1) under simulated solar light, which was superior to ZnO, Co_(3)O_(4) and binary ZnO@Co_(3)O_(4).The internal cavity, exposed active sites, multiple interfaces and constructed p-n heterojunction can facilitate the light harvesting and photoexcited electron transfer. Besides, after introduction of CDs placed in the middle layer between ZnO and Co_(3)O_(4), CDs with excellent photoelectric property further promoted charge separation and migration. This work represents an appealing strategy to construct well-defined photocatalysts for boosting CO_(2) photoreduction.

关键词： Metal-organic framework Photocatalytic CO_(2) reduction Carbon dots p-n heterojunction Sandwich heterostructure

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Modulating the degree of O vacancy defects to achieve selective control of electrochemical CO_(2) reduction products

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Chinese Chemical Letters 2024年第5期35卷 482-486页

作者： Tianbo Jia Lili Wang zhouhao Zhu Baikang Zhu yingtang zhou Guoxing Zhu Mingshan Zhu Hengcong Tao School of Petrochemical Engineering&Environment Zhejiang Ocean UniversityZhoushan 316022China Department of General Practice First Medical CenterChinese PLA General HospitalBeijing 100853China National&Local Joint Engineering Research Center of Harbor Oil&Gas Storage and Transportation Technology Zhoushan 316022China School of Chemistry and Chemical Engineering Jiangsu UniversityZhenjiang 212013China Guangdong Key Laboratory of Environmental Pollution and Health School of EnvironmentJinan UniversityGuangzhou 511443China

Conversion of CO_(2) into high-value products using electrochemical CO_(2) reduction(ECR)technology is an effective way to alleviate global warming and reach carbon neutrality.The oxygen vacancies in heterogenous catalysis are generally considered as a powerful method to enhance the performance of ECR by promoting CO_(2) adsorption and activation.However,the extent of defects in oxygen vacancies-activity relation has rarely been studied.Herein,we prepared Cu-Cd bimetallic catalysts with adjustable oxygen defect degree by controlling the amount of cadmium addition.Fourier transform infrared spectroscopy characterization results reveal that the formation of oxygen vacancies is attributed to the asymmetric stretching of Cu-O by the addition of cadmium.Electrochemical results show that the oxygen defect degree can modulate the selectivity of ECR products.A low degree of oxygen defects(CuO)is generally associated with lower product Faraday efficiency(FE_(C2)/FE_(C1)≈114%),but overabundant oxygen vacancies(CuO_(2.625)-CdO_(0.375))are not entirely favorable to improving ECR activity(FE_(C2)/FE_(C1)≈125%)and single selectivity,while an appropriate degree of oxygen vacancies(CuO_(2.75)-CdO_(0.25))can facilitate the ECR process toward single product selective production(FE_(C2)/FE_(C1)≈296%).The theoretical calculation showed that the O vacancy formed on CuO and the interface between CdO and CuO were conducive to enhancing the formation of ^(*)COOH intermediate and promoting the generation of ethylene products.This study provides a new approach and insight into the selective production of single products for future industrial applications of ECR.

关键词： CO_(2) O-vacancies Bimetallic catalysts Copper oxide Cadmium oxide Selective

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Photoelectrocatalytic hydrogen evolution and synchronous degradation of organic pollutants by pg-C_(3)N_(4)/β-FeOOH S-scheme heterojunction

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Science China(Technological Sciences) 2024年第4期67卷 1238-1252页

作者： LI XiBao HAN Tao zhou yingtang XIE Yu LUO YiDan HUANG JunTong CHEN Zhi DENG Fang School of Materials Science and Engineering Nanchang Hangkong UniversityNanchang 330063China National-Local Joint Engineering Research Center of Heavy Metal Pollutants Control and Resource Utilization Nanchang Hangkong UniversityNanchang 330063China Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316022China

Crafting photoelectrocatalytic materials with robust oxidation-reduction properties for simultaneous hydrogen evolution and pollutant degradation poses a formidable challenge.In this study,a pg-C_(3)N_(4)/β-FeOOH S-scheme heterostructure with a special energy band structure was developed by anchoring porous pg-C_(3)N_(4)on needle shapedβ-FeOOH.Functioning as a hole extraction layer,needle-leaf-likeβ-FeOOH can facilitate efficient hole migration and enhance charge transport.Remarkably,the optimized 0.2-pg-C_(3)N_(4)/β-FeOOH could degrade 78%of ofloxacin(OFLO)in 90 min.The organic pollutants could absorb a large number of holes,which prompted a greater proportion of photogenerated electrons to actively participate in the hydrogen evolution reaction at the cathode.Consequently,the hydrogen production of 0.2-pg-C_(3)N_(4)/β-FeOOH reached 1452.88μmol cm^(-2)h^(-1),exhibiting a notable increase of 61.81-165.12μmol cm^(-2)h^(-1)compared with that in the absence of pollutants.Experimental and theoretical calculation results underscore that this investigation is grounded in a distinctive electron and hole dual channel transfer mechanism.These findings offer novel insights for the future development of S-scheme heterojunction photoelectrocatalytic materials capable of concurrently degrading pollutants and promoting hydrogen evolution.

关键词： photoelectrocatalysis hydrogen evolution degradation synchronous S-scheme heterojunction

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Nanocoating of CsgA protein for enhanced cell adhesion and proliferation

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Chinese Chemical Letters 2023年第4期34卷 154-157页

作者： Chao Yang Dan Li Shaohong Zang yingtang zhou Lei Zhang Zhangfeng Zhong National Engineering Research Center for Marine Aquaculture Institute of Innovation&ApplicationZhejiang Ocean UniversityZhoushan 316022China State Key Laboratory of Southwestern Chinese Medicine Resources School of PharmacyChengdu University of Traditional Chinese MedicineChengdu 611137China Department of Chemical Engineering Waterloo Institute for NanotechnologyUniversity of WaterlooWaterlooON N_(2)L3G1Canada Macao Centre for Research and Development in Chinese Medicine Institute of Chinese Medical SciencesUniversity of MacaoMacao 999078China

Immune rejection, poor biocompatibility and cytotoxicity have seriously stalled the widespread application of biometallic materials. To overcome these problems, biometallic materials with fast and sufficient osseointegration, antibacterial properties and long-term stability have attracted the attention of researchers worldwide. Surface modification is currently used as a general strategy to develop material coatings that will overcome these challenging requirements and achieve the successful performance of implants. In this study, we proposed a substrate surface-modification strategy based on biofilm Csg A proteins that promote rapid cell attachment, proliferation, and stabilization of the cytoskeleton. Csg A-based nano-coating is easy to fabricate and has superior performance, which is expected to expand the application of medical implants.

关键词： Biocompatibility CsgA Fractal-like morphologies Nanocoatings Wound healing

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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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Photo-induced 1,2-aryl migration of 2-chloro-1-arylpropanone under batch and flow conditions:Rapid,scalable and sustainable approach to 2-arylpropionic acids

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Chinese Chemical Letters 2024年第2期35卷 366-369页

作者： Qiao Li Minjie Liu Meifen Jiang Li Wan yingtang Ning Fen-Er Chen College of Chemical Engineering Zhejiang University of TechnologyHangzhou 310014China Engineering Center of Catalysis and Synthesis for Chiral Molecules Fudan UniversityShanghai 200433China Shanghai Engineering Center of Industrial Catalysis for Chiral Drugs Shanghai 200433China Institute of Pharmaceutical Science and Technology Zhejiang University of TechnologyHangzhou 310014China

We report the photo-mediated 1,2-aryl migration of 2‑chloro-1-arylpropanones to 2-arylpropionic acids using HCOONa as an acid scavenger.This pragmatically focused study obviates the multiple-step sequence in the industrially employed,ZnO-promoted rearrangement strategy,and offers rapid access to various 2-arylpropionic acids under environmentally friendly conditions.Furthermore,the successful transfer of this batch photochemistry to a continuous flow platform led to improved scalability and enabled the gram-scale synthesis of loxoprofen.

关键词： Green chemistry Flow chemistry 2-Arylpropionic acids Photo-Favorskii reaction

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Screening promising TM-doped CeO_(2) monolayer for formaldehyde sensor with high sensitivity and selectivity

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Chinese Chemical Letters 2023年第1期34卷 534-538页

作者： zhouhao Zhu Hengcong Tao Jingbin Fu yingtang zhou Jian Guo Chunyang Zhai School of Petrochemical Engineering&Environment Zhejiang Ocean UniversityZhoushan 316022China School of Port and Transportation Engineering Zhejiang Ocean UniversityZhoushan 316022China College of Chemical and Biological Engineering Zhejiang UniversityHangzhou 310058China Key Laboratory of Key Technical Factors in Zhejiang Seafood Health Hazards Zhejiang Ocean UniversityZhoushan 316022China School of Materials Science and Chemical Engineering Ningbo UniversityNingbo 315211China

Developing convenient,fast-response and high-performance formaldehyde detection sensor is significant but challenging.Herein,two CeO_(2) phases(Fm■m and P4_(2)/mnm),three facets(CeO_(2)(100),CeO_(2)(110)and CeO_(2)(111))and three adsorption sites(top,bridge and hollow)are selected as substrate to interact with formaldehyde.Twenty-eight candidated transition metals(TM)are doped on CeO_(2) surfaces to investigate the performance of detecting formaldehyde by density functional theory.It shows that(i)CeO_(2) in a cubic fluorite structure with the space group Fm■m is suitable for formaldehyde adsorption compared with P4_(2)/mnm;(ii)TM-CeO_(2)(100)(TM=Au,Hf,Nb,Ta,Zr)are considered as candidated materials to absorb formaldehyde ascribed to lower adsorption energies.The d-band center,partial density of states,charge density difference and electron localization function are employed to clarify the mechanism of TM-doped CeO_(2) improving the performance of formaldehyde adsorption.It obviously displays that TM doped CeO_(2)(100)changes the d orbit and rearranges electrons resulting in the superior ability to the adsorbed formaldehyde.This work provides theoretical guidance and experimental motivation for the development of novel formaldehyde sensor based on metal oxide semiconductor materials.

关键词： Cerium oxide Density functional theory Formaldehyde Metal doping

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Compositional engineering of HKUST-1/sulfidized NiMn-LDH on functionalized MWCNTs as remarkable bifunctional electrocatalysts for water splitting

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Carbon Energy 2023年第12期5卷 1-20页

作者： Mengshan Chen Reza Abazari Soheila Sanati Jing Chen Mingyuzhi Sun Cunhong Bai Alexander M.Kirillov yingtang zhou Guangzhi Hu Zhejiang Key Laboratory of Petrochemical Environmental Pollution Control National Engineering Research Center for Marine AquacultureMarine Science and Technology CollegeZhejiang Ocean UniversityZhoushanChina Department of Chemistry Faculty of ScienceUniversity of MaraghehMaraghehIran State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering College of Chemistry and Chemical EngineeringNingxia UniversityYinchuanChina Departamento de Engenharia Química Centro de Química EstruturalInstitue of Molecular SciencesInstituto Superior TécnicoUniversidade de LisboaLisbonPortugal School of Ecology and Environmental Science Institute for Ecological Research and Pollution Control of Plateau LakesYunnan UniversityKunmingChina

Water-splitting reactions such as the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)typically require expensive noble metal-based electrocatalysts.This has motivated researchers to develop novel,cost-effective electrocatalytic systems.In this study,a new multicomponent nanocomposite was assembled by combining functionalized multiwalled carbon nanotubes,a Cu-based metal–organic framework(MOF)(HKUST-1 or HK),and a sulfidized NiMn-layered double hydroxide(NiMn-S).The resulting nanocomposite,abbreviated as MW/HK/NiMn-S,features a unique architecture,high porosity,numerous electroactive Cu/Ni/Mn sites,fast charge transfer,excellent structural stability,and conductivity.At a current density of 10 mA cm-2,this dual-function electrocatalyst shows remarkable performance,with ultralow overpotential values of 163 mV(OER)or 73 mV(HER),as well as low Tafel slopes(57 and 75 mV dec-1,respectively).Additionally,its high turnover frequency values(4.43 s-1 for OER;3.96 s-1 for HER)are significantly superior to those of standard noble metal-based Pt/C and IrO2 systems.The synergistic effect of the nanocomposite's different components is responsible for its enhanced electrocatalytic performance.A density functional theory study revealed that the multi-interface and multicomponent heterostructure contribute to increased electrical conductivity and decreased energy barrier,resulting in superior electrocatalytic HER/OER activity.This study presents a novel vision for designing advanced electrocatalysts with superior performance in water splitting.Various composites have been utilized in water-splitting applications.This study investigates the use of the MW/HK/NiMn-S electrocatalyst for water splitting for the first time to indicate the synergistic effect between carbon-based materials along with layered double hydroxide compounds and porous compounds of MOF.The unique features of each component in this composite can be an interesting topic in the field of water splitting.

关键词： bifunctional electrocatalyst electroactive sites multicomponent synergic effect water splitting

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Modulation of photocatalytic activity of SrBi_(2)Ta_(2)O_(9)nanosheets in NO removal by tuning facets exposure

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Journal of Materials Science & Technology 2022年第27期122卷 91-100页

作者： Nan Li Qiuhui Zhu Guimei Liu Qi Zhao Haiqin Lv Mingzhe Yuan Qingguo Meng yingtang zhou Jingkun Xu Chuanyi Wang School of Environmental Science and Engineering Shaanxi University of Science and TechnologyXi’an 710021China Guangzhou Institute of Industrial Intelligence(GIII) Guangzhou 511400China National Engineering Research Center for Marine Aquaculture Marine Science and Technology CollegeZhejiang Ocean UniversityZhoushan 316004China Flexible Electronics Innovation Institute(FEII) Jiangxi Science&Technology Normal UniversityNanchang 330006China

Photocatalysts with exposure of different crystal facets often show great differences in their photocatalytic activities due to differences in surface atomic arrangement and coordination.Thus,the actual photoreaction mechanism of a specific crystal facet in photocatalysis deserves to be explored.In this paper,as a case study,Sr Bi_(2)Ta_(2)O_(9)photocatalyst with preferential facet exposure was explored for the photocatalytic removal of NO at a ppb level.The efficiency of NO removal was remarkably improved by tuning the crystal exposure facet with high(200)facet exposure ratio.Optimized exposure of(200)crystal facet in Sr Bi_(2)Ta_(2)O_(9)(SBT)by thermal calcination at 800℃(SBT-800)leads to the highest NO removal activity of51%under a 300 W Xe lamp for 20 min;under visible light,SBT 800 achieves a 5-fold enhancement in NO removal efficiency compared to its counterpart,SBT-900.Active species capture experiments prove that the superoxide radical·O_(2)-is the main active species for the photocatalytic removal of NO,and surface selective deposition experiments conclude that(200)is the main electron-rich crystal plane,based on which the results of density functional theory(DFT)computation reveal the Bi O terminated nature of(001)crystal plane,where the models with both Bi O and Ta O terminated(001)planes were created and computated.Mechanistic study reveals that Sr Bi_(2)Ta_(2)O_(9)with a larger exposure of(200)facet provides more active reduction sites,thereby reducing more O_(2)to·O_(2)-,which further oxidizes the adsorbed NO to NO_(2)-/NO_(3)-.The present work underlines the role of facet tuning in the photoactivity modulation for NO removal photocatalytically.

关键词： SrBi_(2)Ta_(2)O_(9) NO removal Facet exposure Photocatalysis DFT computation

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