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Rational design of vitamin C/defective carbon van der Waals heterostructure for enhanced activity,durability and storage stability toward oxygen reduction reaction

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Journal of Energy Chemistry 2024年第1期88卷 103-111,I0003页

作者： Ruiqi Cheng Kaiqi Li Huanxin Li Tianshuo Zhao Yibo Wang Qingyue Xue Jiao Zhang Chaopeng Fu Shanghai Key Laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Department of Chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK

Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air ***,the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage,leading to rapid degradation of ***,we design a van der Waals heterostructure comprised of vitamin C(VC)and defective carbon(DC)to not only boost the activity but also enhance the durability and storage stability of the DC-VC *** formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation,thus significantly enhancing the electrochemical durability and storage anti-aging ***,the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the *** findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory *** is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up,and the ORR performance of the largely produced electrocatalyst is demonstrated to be very ***,the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.

关键词： Van der Waals heterostructure Oxygen reduction reaction Stability Scalable production Aluminum-air battery

In-situ transformed Mott-Schottky heterointerface in silver/manganese oxide nanorods boosting oxygen reduction,oxygen evolution,and hydrogen evolution reactions

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Nano Research 2024年第5期17卷 3622-3632页

作者： Ruiqi Cheng Kaiqi Li Huanxin Li Fengzhan Sun Xiaoqian He Tianshuo Zhao Jiao Zhang Chaopeng Fu Shanghai Key Laboratory of Advanced High-temperature Materials and Precision Forming School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China Christopher Ingold Laboratory Department of ChemistryUniversity College LondonLondon WC1H 0AJUK Department of Chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK Center of Hydrogen Science School of Materials Science and EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The development of non-platinum group metal(non-PGM)and efficient multifunctional electrocatalysts for oxygen reduction reaction(ORR),oxygen evolution reaction(OER),and hydrogen evolution reaction(HER)with high activity and stability remains a great ***,by in-situ transforming silver manganese composite oxide heterointerface into boosted Mott-Schottky heterointerface through a facile carbon reduction strategy,a nanorod-like silver/manganese oxide with superior multifunctional catalytic activities for ORR,OER and HER and stability was *** nanorod-like silver/manganese oxide with Mott-Schottky heterointerface(designated as Ag/Mn_(3)O_(4))exhibits an ORR half-wave potential of 0.831 V(***)in 0.1 M KOH,an OER overpotential of 338 mV and a HER overpotential of 177 mV at the current density of 10 mA·cm^(-2)in 1 M KOH,contributing to its noble-metal benchmarks comparable performance in aqueous aluminum-air(Al-air)battery and laboratorial overall water splitting electrolytic ***,in-situ electrochemical Raman and synchrotron radiation spectroscopic measurements were conducted to further illustrate the catalytic mechanism of Ag/Mn_(3)O_(4)Mott-Schottky heterointerface towards various electrocatalytic *** the heterointerface,the Ag phase serves as the electron donor and the active phase for ORR and HER,while the Mn_(3)O_(4)phase serves as the electron acceptor and the active phase for OER,*** work deepens the understanding of the Mott-Schottky effect on electrocatalysis and fills in the gap in fundamental physical principles that are behind measured electrocatalytic activity,which offers substantial implications for the rational design of cost-effective multifunctional electrocatalysts with Mott-Schottky effect.

关键词： heterointerface electron donor-acceptor pair electrocatalyst Al-air battery water splitting

Ultra-thin Oxide Films on SiO_2: An STM Study of Their Thermal Stability in the Presence of Au Deposit

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Chemical Research in Chinese Universities 2002年第2期18卷 124-129页

作者： Jun Wang CEJMitchell RGEgdell JSFoord Physical and Theoretical Chemistry Laboratory South Parks RoadOxford OX13QZUK Inorganic Chemistry Laboratory South Parks RoadOxford OX13QRUK

The annealing of Au particles deposited onto the ultrathin layers of SiO 2 on Si(111) has been studied in real time with a high temperature scanning tunnelling microscopy. Annealing did not create significant changes to the morphology of the surface until the surface was heated up to more than 920 K when the gold particles started to display a preference for the step edge. Further heating caused the decomposition of the oxide layer with the formation of voids on the surface in the surface step edge area. Comparison between the gold assisted oxide decomposition and pure oxide decomposition indicates that the two decomposition routes proceed with different mechanisms.

关键词： Scanning tunnelling microscopy Silicon oxide Gold Surface diffusion Surface structure Morphology Roughness and topology Oxidation Decomposition

Boric Acid-Assisted Pyrolysis for High-Loading Single-Atom Catalysts to Boost Oxygen Reduction Reaction in Zn-Air Batteries

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Energy & Environmental Materials 2024年第2期7卷 102-110页

作者： Chenxi Xu Jiexing Wu Liang Chen Yi Gong Boyang Mao Jincan Zhang Jinhai Deng Mingxuan Mao Yan Shi Zhaohui Hou Mengxue Cao Huanxin Li Haihui Zhou Zhongyuan Huang Yafei Kuang State Key Laboratory for Chemo/Biosensing and Chemometrics and College of Chemistry and Chemical Engineering Hunan UniversityChangsha 410082China School of Chemistry and Chemical Engineering Key Laboratory of Hunan Province for Advanced Carbon-based Functional MaterialsHunan Institute of Science and TechnologyYueyang 414006China Advanced Technology Institute University of SurreyGuildford Surrey GU27XHUK Department of Engineering University of Cambridge9 JJ Thomson AvenueCambridge CB30FAUK King's College London London SE11ULUK Department of Electrical and Electronic Engineering Imperial College LondonLondon SW72AZUK College of Materials and Metallurgy Guizhou UniversityGuiyang 550025China Department of Chemistry Physical&Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OX13QZUK

The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production of high-loading SACs is still ***,a facile and green boron acid(H_(3)BO_(3))-assisted pyrolysis strategy is put forward to synthesize SACs by only using chitosan,cobalt salt and H_(3)BO_(3)as precursor,and the effect of H_(3)BO_(3)is deeply *** results show that molten boron oxide derived from H_(3)BO_(3)as ideal high-temperature carbonization media and blocking media play important role in the synthesis *** a result,the acquired Co/N/B tri-doped porous carbon framework(Co-N-B-C)not only presents hierarchical porous structure,large specific surface area and abundant carbon edges but also possesses high-loading single Co atom(4.2 wt.%),thus giving rise to outstanding oxygen catalytic *** employed as a catalyst for air cathode in Zn-air batteries,the resultant Co-N-B-C catalyst shows remarkable power density and long-term ***,our work gains deep insight into the role of H_(3)BO_(3)and provides a new avenue to synthesis of high-performance SACs.

关键词： boric acid oxygen reduction reaction single-atom catalysts Zn-air batteries

Applications of Pattern Recognition in Drug Discovery

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Chemical Research in Chinese Universities 2002年第2期18卷 107-108页

作者： W. Graham Richards Department of Chemistry, University of Oxford, Central Chemistry, south parks road, Oxford OX1 3QH, UK Department of Chemistry University of Oxford Central Chemistry South Parks Road 英国 Oxford

This is a brief account of the plenary talk given to the meeting of the Chinese Society of Chemical Science and Technology held in Oxford on 6 October 2001. The talk covered the application of pattern recognition techniques to discover molecules which will bind to the binding sites of proteins. Three situations were considered: the structure of the protein being unknown; the structure known but the binding site unknown; and finally, and this is the most important case for the future, both the structure and nature of the target site available in atomic detail. For this case we have developed a massively distributed computer program using a screensaver which now involves over one million personal computers, including over a thousand in China. The project will involve the screening of 3 5 billion small molecules against 16 protein targets, all of which are implicated in the process of cancer.

关键词： Pattern recognition Drug Protein Gene Binding site

Methane Dry Reforming over Alumina Supported Co Catalysts

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Chemical Research in Chinese Universities 2004年第4期20卷 457-461页

作者： Sergio L. González Cortés Malcolm L. H. Green Inorganic Chemistry Laboratory University of OxfordInorganic Chemistry Laboratory University of Oxford South Parks Road OX1 3QR UKSouth Parks Road OX1 3QR UK

A series of Co/γ-Al_2O_3 catalysts were prepared with the impregnation method and characterized by means of the BET specific surface area, X-ray diffraction(XRD), thermogravimetric analysis(TGA) and Laser Raman spectroscopy. The Co/γ-Al_2O_3 catalysts were activated by using H_2, 20%CH_4/H_2 or CH_4, respectively. There was no obvious difference between the activities of the Co/γ-Al_2O_3 catalyst activated by using the different activation methods for methane dry reforming. The catalytic properties of the Co/γ-Al_2O_3 catalysts with different Co loadings were also investigated. The optimized Co loading for the Co/γ-Al_2O_3 catalyst pretreated with 20% CH_4/H_2 is around 12%(mass fraction).

关键词： Methane dry reforming Alumina supported cobalt catalysts Catalytic deactivation

Tungsten Promoted Ni/Al_2O_3 Catalysts for Carbon Dioxide Reforming of Methane to Synthesis Gas

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Chemical Research in Chinese Universities 2004年第4期20卷 470-477页

作者： Thomas Suhartanto Andrew P. E. York Malcolm L. H. Green Wolfson Catalysis Centre Inorganic Chemistry Laboratory University of OxfordWolfson Catalysis Centre Inorganic Chemistry Laboratory University of OxfordWolfson Catalysis Centre Inorganic Chemistry Laboratory University of Oxford South Parks Road Oxford OX1 3QR UKSouth Parks Road Oxford OX1 3QR UKSouth Parks Road Oxford OX1 3QR UK

A series of tungsten promoted alumina supported nickel catalysts has been prepared for the carbon dioxide reforming of methane to synthesis gas. The catalysts have been characterized by means of XRD, TEM, and Laser Raman spectroscopy. It is shown that the addition of tungsten to the nickel catalyst can stabilize the catalyst and increase the resistance to carbon deposition. Adding a suitable amount of tungsten can also increase the catalyst activity to be close to that of supported noble metal catalysts. The carburisation of the tungsten modified nickel catalyst decreases the catalyst activity at lower reaction temperatures(<1123K), but has no effect on the catalyst performance at higher reaction temperatures. The alumina supported nickel catalyst modified by 0.67%(mass fraction) WO_3 has the equivalent equilibrium constant of the dry reforming reaction to that of alumina supported 5%(mass fraction) Ru at 873 K, and also has a lower activation energy for dry reforming than the latter.

关键词： Nickel catalyst Tungsten modifier CO_2 reforming Methane Syngas

Electro-oxidation of hydrazine shows marcusian electron transfer kinetics

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Science China Chemistry 2021年第2期64卷 322-329页

作者： Ruiyang Miao Lifu Chen Richard G Compton Department of Chemistry Physical and Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxfordOX13QZUK

Although hydrazine(N2 H4) oxidation in an electrochemical environment has been of great interest for years,its intrinsic electron transfer kinetics remain *** report that the phenomenological Butler-Volmer(BV) theory is not appropriate for interpreting the process of hydrazine oxidation for which an astonishingly wide range of transfer coefficients,Tafel slopes and diffusion coefficient have been previously *** Tafel analysis for voltammetry recorded at Glassy Carbon(GC)electrodes reveals a strong potential dependence of the anodic transfer coefficient,consistent with the symmetric Marcus-Hush(sMH) *** to the relationship β=λ+FEf^0/2λ-F/2λ E,the reorganization energy(0.35±0.07 eV) and an approximate formal potential of the rate-determining first electron transfer were successfully extracted from the voltammetric responses.

关键词： hydrazine electrode kinetics transfer coefficient Butler-Volmer theory Marcus-Hush theory

Substrate mediated dissolution of redox active nanoparticles;electron transfer over long distances

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Nano Research 2022年第1期15卷 429-437页

作者： Ruo-Chen Xie Christopher Batchelor-McAuley Minjun Yang Richard G.Compton Department of Chemistry Physical and Theoretical Chemistry LaboratoryUniversity of OxfordSouth Parks RoadOxford OXl 3QZUK

Reflective dark field microscopy is used to observe the decrease in the light scattered from Ag nanoparticles immobilised on differing solid *** nanoparticles are exposed to solutions containing halide ions,both at open circuit and under potentiostatic control,leading to the loss of the *** coupling optical and electrochemical techniques the physical origin of this transformation is demonstrated to be the electrochemical dissolution of the metal nanoparticles driven by electron transfer to ultra-trace dissolved *** dissolution kinetics of the surface-supported metal nanoparticles is compared on four substrate materials(i.e.,glass,indium titanium oxide,glassy carbon and platinum)with different electrical *** three conductive substrates catalyse the redox-driven dissolution of Ag nanoparticles with the electrons transferred from the nanoparticles,via the macroscopic electrode to the dioxygen electron acceptor.

关键词： substrate electrocatalysis oxidative dissolution metal nanoparticles optical microscopy electrochemistry