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Achieving highly selective electrochemical CO_(2) reduction to C_(2)H_(4) on Cu nanosheets

Journal of Energy Chemistry 2023年第4期79卷 312-320页

作者： Huan Xie Ruikuan Xie Zhiyuan Zhang Yongyu Pang Yuting Luo Jiong Li Bilu Liu maria-magdalena titirici Guoliang Chai State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002FujianChina Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Materials Science and EngineeringNanjing Forestry UniversityNanjing 210037JiangsuChina Shenzhen Geim Graphene Center(SGC) Tsinghua-Berkeley Shenzhen Institute(TBSI)and Tsinghua Shenzhen International Graduate School(TSIGS)Tsinghua UniversityShenzhen 518055GuangdongChina School of Chemical Science University of Chinese Academy of SciencesBeijing 100049China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research Institute Chinese Academy of SciencesShanghai 201210China Department of Chemical Engineering Imperial College LondonSW72AZUK

The conversion of CO_(2)into value-added chemicals coupled with the storage of intermittent renewable electricity is attractive.CuO nanosheets with an average size and thickness of~30 and~20 nm have been developed,which are in situ reduced into Cu nanosheets during electrochemical CO_(2)reduction reaction(ECO_(2)RR).The derived Cu nanosheets demonstrate much higher selectivity for C2H4production than commercial CuO derived Cu powder,with an optimum Faradaic efficiency of 56.2%and a partial current density of C_(2)H_(4)as large as 171.0 mA cm^(-2)in a gas diffusion flow cell.The operando attenuated total reflectance-Fourier transform infrared spectra measurements and density functional theory simulations illustrate that the high activity and selectivity of Cu nanosheets originate from the edge sites on Cu nanosheets with a coordinate number around 5(4–6),which facilitates the formation of^(*)CHO rather than^(*)COH intermediate,meanwhile boosting the C-C coupling reaction of^(*)CO and^(*)CHO intermediates,which are the critical steps for C_(2)H_(4)formation.

关键词： Electrochemical CO_(2)reduction Cu nanosheets C_(2)H_(4) High selectivity Coordination number

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A review of nanocarbons in energy electrocatalysis: Multifunctional substrates and highly active sites

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Journal of Energy Chemistry 2017年第6期26卷 1077-1093页

作者： Cheng Tang maria-magdalena titirici Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical Engineering Tsinghua University Queen Mary University of London School of Engineering and Materials Science

Nanocarbons are of progressively increasing importance in energy electrocatalysis, including oxygen reduction, oxygen evolution, hydrogen evolution, COreduction, etc. Precious-metal-free or metal-free nanocarbon-based electrocatalysts have been revealed to potentially have effective activity and remarkable durability, which is promising to replace precious metals in some important energy technologies,such as fuel cells, metal–air batteries, and water splitting. In this review, rather than overviewing recent progress completely, we aim to give an in-depth digestion of present achievements, focusing on the different roles of nanocarbons and material design principles. The multifunctionalities of nanocarbon substrates(accelerating the electron and mass transport, regulating the incorporation of active components,manipulating electron structures, generating confinement effects, assembly into 3 D free-standing electrodes) and the intrinsic activity of nanocarbon catalysts(multi-heteroatom doping, hierarchical structure,topological defects) are discussed systematically, with perspectives on the further research in this rising research field. This review is inspiring for more insights and methodical research in mechanism understanding, material design, and device optimization, leading to a targeted and high-efficiency development of energy electrocatalysis.

关键词： Nanocarbon Energy electrocatalysis Oxygen reduction Oxygen evolution Hydrogen evolution CO_2 reduction Electron structure Strong coupling effect Hierarchical structure Doping Defect Metal–air battery Fuel cell Water splitting

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Achieving high initial Coulombic efficiency for competent Na storage by microstructure tailoring from chiral nematic nanocrystalline cellulose

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Carbon Energy 2022年第5期4卷 914-923页

作者： Fei Xie Zhen Xu Zhenyu Guo Anders CSJensen Jingyu Feng Hui Luo Feixiang Ding Yaxiang Lu Yong-Sheng Hu maria-magdalena titirici Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijingChina Department of Chemical Engineering Imperial College LondonLondonUK School of Physical and Chemical Sciences Queen Mary University of LondonLondonUK Huairou Division Institute of PhysicsChinese Academy of SciencesBeijingChina Yangtze River Delta Physics Research Center Co. Ltd.LiyangChina College of Materials Science and Optoelectronics Technology University of Chinese Academy of SciencesBeijingChina

Although it has been proven that porous,heteroatomic,and defective structures improve Na storage performance,they also severely affect the initial Coulombic efficiency(ICE)due to the huge irreversible capacity in the first cycle,which always limits the practical application of carbon anodes in commercial Na-ion batteries(NIBs).Here,we show the successful synthesis of nanocrystalline cellulose and the derivative hard carbons.A series of treatments including acid hydrolysis,hydrothermal carbonization,and hightemperature pyrolysis help tune the pores,heteroatoms,and defects to achieve an optimized balance between superior ICE and reversible capacity of up to 90.4%and 314 mAh g^(−1).This study highlights that tailoring the electrode microstructure could be an important strategy in the future design of carbonaceous anode materials for high-performance Na-ion batteries.

关键词： hard carbon microstructure Na storage nanocrystalline cellulose

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Sulphur-doped ordered mesoporous carbon with enhanced electrocatalytic activity for the oxygen reduction reaction

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Journal of Energy Chemistry 2016年第4期25卷 566-570页

作者： Liping Wang Weishang Jia Xiaofeng Liu Jingze Li maria magdalena titirici State Key Laboratory of Electronic Thin Films and Integrated Devices University of Electronic Science and Technology of China School of Materials Science and Engineering Zhejiang University School of Materials Science and Engineering Queen Mary University of London Materials Research Institute Queen Mary University of London

Metal-free, heteroatom functionalized carbon-based catalysts have made remarkable progress in recent years in a wide range of applications related to energy storage and energy generation. In this study, high surface area mesoporous ordered sulphur doped carbon materials are obtained via one-pot hydrothermal synthesis of carbon/SBA-15 composite after removal of in-situ synthesized hard template SiO2. 2-thiophenecarboxy acid as sulphur source gives rise to sulphur doping level of 5.5 wt%. Comparing with pristine carbon, the sulphur doped mesoporous ordered carbon demonstrates improved electro-catalytic activity in the oxygen reduction reaction in alkaline solution. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Mesoporous ordered carbon Oxygen reduction reaction Electrocatalyst Heteroatom doping In-situ synthesis

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Hard carbon derived from rice husk as low cost negative electrodes in Na-ion batteries

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Journal of Energy Chemistry 2019年第2期28卷 17-22页

作者： maria K.Rybarczyk Yunming Li Mo Qiao Yong-Sheng Hu maria-magdalena titirici Marek Lieder Gdansk University of Technology Chemical Faculty Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesNational Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of Sciences Queen Mary University London School of Materials Science & Engineering

Here,we report the synthesis of hard carbon materials(RH) made from natural rice husk through a single pyrolysis process and their application as an anode in sodium-ion batteries.The studies show that the electrochemical properties of RHs are affected by the treatment temperatures,which determine the materials morphology,in particular,their degree of graphitization and extent of continuous channels(nanovoids).The latter are accessible to sodium ions and significantly contribute to charge storage capacity of the produced anodes.The RHs obtained at 1600 °C deliver the highest reversible capacity of276 mAh g^(-1) mainly due to insertion of sodium ions into the nanovoids.This work deepens the basic understanding of the influence of the carbonization temperature on the sodium storage mechanism.

关键词： Nanovoids in rice husk Sustainable energy storage Na-ion batteries

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Disordered carbon anodes for Na-ion batteries—quo vadis?

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Science China Chemistry 2021年第10期64卷 1679-1692页

作者： Fei Xie Zhen Xu Zhenyu Guo Yaxiang Lu Liquan Chen maria-magdalena titirici Yong-Sheng Hu Key Laboratory for Renewable Energy Beijing Key Laboratory for New Energy Materials and DevicesBeijing National Laboratory for Condensed Matter PhysicsInstitute of PhysicsChinese Academy of SciencesBeijing 100190China Department of Chemical Engineering Imperial College LondonLondon SW72AZUK

Na-ion batteries(NIBs)are gradually attracting much attention as an alternative to lead-acid batteries and supplement to Li-ion batteries(LIBs)owing to the abundant Na resources and excellent cost-effectiveness.Since the most commonly used graphite as an anode material in LIBs cannot be inherently used in NIBs,tremendous efforts have been made to advance the fundamental understanding and design of suitable anode materials for NIBs,including the improvement of Na storage capacity and the study on Na storage mechanisms.According to all these studies,disordered carbons are now the most promising anode candidates for NIBs.In this review,we discuss the current challenges and remaining problems to be solved in the area of disordered carbon anode materials for NIBs and provide future insights and research directions.

关键词： disordered carbon anode Na-ion batteries

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Bio-inspired carbon electro-catalysts for the oxygen reduction reaction

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Journal of Energy Chemistry 2016年第2期25卷 226-233页

作者： Kathrin Preuss Vasanth Kumar Kannuchamy Adam Marinovic Mark Isaacs Karen Wilson Isaac Abrahams maria-magdalena titirici School of Engineering and Materials Science Queen Mary University of London Materials Research Institute Queen Mary University of London European Bioenergy Research Institute Aston University School of Biological and Chemical Sciences Queen Mary University of London

We report the synthesis, characterisation and catalytic performance of two nature-inspired biomassderived electro-catalysts for the oxygen reduction reaction in fuel cells. The catalysts were prepared via pyrolysis of a real food waste（lobster shells） or by mimicking the composition of lobster shells using chitin and CaCO3 particles followed by acid washing. The simplified model of artificial lobster was prepared for better reproducibility. The calcium carbonate in both samples acts as a pore agent, creating increased surface area and pore volume, though considerably higher in artificial lobster samples due to the better homogeneity of the components. Various characterisation techniques revealed the presence of a considerable amount of hydroxyapatite left in the real lobster samples after acid washing and a low content of carbon（23%）, nitrogen and sulphur（〈1%）, limiting the surface area to 23 m^2/g, and consequently resulting in rather poor catalytic activity. However, artificial lobster samples, with a surface area of ≈200 m^2/g and a nitrogen doping of 2%, showed a promising onset potential, very similar to a commercially available platinum catalyst, with better methanol tolerance, though with lower stability in long time testing over 10,000 s.

关键词： Carbonisation Biomass-derived carbons Oxygen reduction reaction Fuel cells Electro-catalysis

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A Review of Advanced Energy Materials for Magnesium–Sulfur Batteries

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Energy & Environmental Materials 2018年第3期1卷 100-112页

作者： Long Kong Chong Yan Jia-Qi Huang Meng-Qiang Zhao maria-magdalena titirici Rong Xiang Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijing 100084China Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijing 100081China Department of Physics and Astronomy University of Pennsylvania209 South33rd StreetPhiladelphia PA 19104USA School of Engineering and Materials Science Queen Mary University of LondonMile End RoadE14NSLondon UK Department of Mechanical Engineering The University of TokyoTokyo 113-8656Japan

Magnesium–sulfur batteries promise high volumetric energy density,enhanced safety,and low cost for electrochemical energy storage.The current obstacles to practical applications of reliable magnesium–sulfur batteries are finding electrolytes that can meet a multitude of rigorous requirements along with efficient sulfur cathodes and magnesium anodes.This review highlights recent advances in designing better electrolytes,cathodes,and anodes.A suitable electrolyte for magnesium-sulfur batteries should allow to reversibly electroplate/strip divalent magnesium ions and should be compatible with the sulfur cathode and the other cell’s components.

关键词： electrolyte energymaterials magnesiumanode magnesium-sulfur batteries sulfur cathode

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A review of rechargeable batteries for portable electronic devices

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InfoMat 2019年第1期1卷 6-32页

作者： Yeru Liang Chen-Zi Zhao Hong Yuan Yuan Chen Weicai Zhang Jia-Qi Huang Dingshan Yu Yingliang Liu maria-magdalena titirici Yu-Lun Chueh Haijun Yu Qiang Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijingChina College of Materials and Energy South China Agricultural UniversityGuangzhouChina School of Chemical and Biomolecular Engineering The University of SydneySydneyNew South WalesAustralia Advanced Research Institute of Multidisciplinary Science Beijing Institute of TechnologyBeijingChina Key Laboratory for Polymeric Composite and Functional Materials Ministry of EducationSchool of ChemistrySun Yat-sen UniversityGuangzhouChina School of Engineering and Materials Science Queen Mary University of LondonLondonUnited Kingdom Department of Materials Science and Engineering National Tsing Hua UniversityHsinchuTaiwanROC College of Materials Science and Engineering Key Laboratory of Advanced Functional MaterialsMinistry of EducationBeijing University of TechnologyBeijingChina

Portable electronic devices(PEDs)are promising information-exchange platforms for real-time responses.Their performance is becoming more and more sensitive to energy consumption.Rechargeable batteries are the primary energy source of PEDs and hold the key to guarantee their desired performance stability.With the remarkable progress in battery technologies,multifunctional PEDs have constantly been emerging to meet the requests of our daily life conveniently.The ongoing surge in demand for high-performance PEDs inspires the relentless pursuit of even more powerful rechargeable battery systems in turn.In this review,we present how battery technologies contribute to the fast rise of PEDs in the last decades.First,a comprehensive overview of historical advances in PEDs is outlined.Next,four types of representative rechargeable batteries and their impacts on the practical development of PEDs are described comprehensively.The development trends toward a new generation of batteries and the future research focuses are also presented.

关键词： electrochemical energy storage information material portable electronic device rechargeable battery

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Electrospinning as a route to advanced carbon fibre materials for selected low-temperature electrochemical devices:A review

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Journal of Energy Chemistry 2021年第8期30卷 492-529,I0011页

作者： Yue Wen Matt D.R.Kok Jorge Pavel Victoria Tafoya Ana BJorge Sobrido Ellsworth Bell Jeff T.Gostick Servann Herou Philipp Schlee maria-magdalena titirici Dan J.L.Brett Paul R.Shearing Rhodri Jervis The Electrochemical Innovation Lab Dept.of Chemical EngineeringUniversity College LondonTorrington PlaceWC1E 7JE LondonUK Queen Mary University of London School of Engineering and Materials ScienceMile End RoadE14NS LondonUK Department of Chemical Engineering University of WaterlooWaterlooCanada Department of Chemical Engineering Imperial College LondonSouth Kensington CampusSW72AZ LondonUK

Electrospinning has been proven as a highly versatile fabrication method for producing nano-structured fibres with controllable morphology,of both the fibres themselves and the void structure of the mats.Additionally,it is possible to use heteroatom doped polymers or to include catalytic precursors in the electrospinning solution to control the surface properties of the fibres.These factors make it an ideal method for the production of electrodes and flow media for a variety of electrochemical devices,enabling reduction in mass transport and activation overpotentials and therefore increasing efficiency.Moreover,the use of biomass as a polymer source has recently gained attention for the ability to embed sustainable principles in the materials of electrochemical devices,complementing their ability to allow an increase in the use of renewable electricity via their application.In this review,the historical and recent developments of electrospun materials for application in redox flow batteries,fuel cells,metal air batteries and supercapacitors are thoroughly reviewed,including an overview of the electrospinning process and a guide to best practice.Finally,we provide an outlook for the emerging use of this process in the field of electrochemical energy devices with the hope that the combination of tailored microstructure,surface functionality and computer modelling will herald a new era of bespoke functional materials that can significantly improve the performance of the devices in which they are used.

关键词： Electrospinning Redox flow batteries Fuel cells Metal-air batteries Supercapacitors

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