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Electrocatalytic CO_(2) reduction to C_(2)H_(4): From lab to fab

Journal of Energy Chemistry 2024年第3期90卷 540-564,I0012页

作者： Zeyu Guo Fabao Yang Xiaotong Li Huiwen Zhu Hainam Do Kam Loon Fow Jonathan D.Hirst Tao wu Qiulin Ye Yaqi Peng Hao Bin wu angjian wu Mengxia Xu Department of Chemical and Environmental Engineering and New Materials InstituteUniversity of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina Key Laboratory of Carbonaceous Waste Processing and Process Intensification of Zhejiang Province University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina Nottingham Ningbo China Beacons of Excellence Research and Innovation Institute University of Nottingham Ningbo ChinaNingbo 315100ZhejiangChina State Key Laboratory of Clean Energy Utilization Department of Energy EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon and Advanced Semiconductor Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina School of Chemistry University of NottinghamUniversity ParkNottingham NG72RDUK Baima Lake Laboratory Hangzhou 310053ZhejiangChina

The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon neutrality.Among these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical industry.Accordingly,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer devices.Subsequently,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial scenarios.Additionally,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market potential.The review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) process.The insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.

关键词： CO_(2) electroreduction reaction Ethylene Gas diffusion electrode Machine learning Density functional theory Techno-economic analysis

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Novel development of VO_(x)-CeO_(x)-WO_(x)/TiO_(2) catalyst for low-temperature catalytic oxidation of chloroaromatic organics

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Waste Disposal and Sustainable Energy 2022年第4期4卷 259-269页

作者： Yunfeng Ma Jianwen Lai Jiayao wu Xiaoqing Lin Hong Yu Hao Zhang angjian wu Jisheng Long Xiaodong Li State Key Laboratory for Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou310027China Shanghai SUS ENVIRONMENT Co. LTDShanghai201703China

A novel selective catalytic reduction(SCR)catalyst with high catalytic activity on chloroaromatic organics at lower temperatures(160-180℃)is critical for municipal solid waste incineration(MSWI)plants.This study prepares a series of honeycomb-type VO_(x)/TiO_(2) catalysts and finally develops a new low-temperature catalyst with high catalytic activity in eliminating chloroaromatic organics.Based on the conversion efficiency(CE)of 1,2-dichlorobenzene(1,2-DCB)and CO_(2) selectivity,the optimal VO_(x) content of 4.06%(in weight)in VO_(x)/TiO_(2) catalyst is first confirmed.By modifying CeO_(x) and WO_(x),a novel honeycomb-type catalyst of VO_(x)-CeO_(x)-WO_(x)/TiO_(2) achieves the highest CE(93.1%-93.6%)and CO_(2) selectivity(40.9%-60.7%)at 150-200℃.It was found that the CeO_(x) and WO_(x) can improve the catalytic activity by enriching the surface content of V and O,increasing the proportion of V5+and Osurf,enlarging the supply source of reactive oxygen species and their storage capacity,and accelerating the redox cycle of VO_(x),CeO_(x),WO_(x),and reactive oxygen species.This study can guide the development of monolithic low-temperature catalysts with high catalytic activity in eliminating chloroaromatic organics in MSWI flue gas.

关键词： VO_(x)/TiO_(2)catalysts Honeycomb catalysts Catalytic activity 1,2-dichlorobenzene Modification of CeO_(x)and WOx

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Zeolite-mediated hybrid Cu^(+)/Cu~0 interface for electrochemical nitrate reduction to ammonia

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Journal of Energy Chemistry 2023年第12期87卷 136-143,I0005页

作者： Jiabao Lv angjian wu Liang Wang Yunhao Zhong Zhihao Zeng Qunxing Huang Xiaoqing Lin Hao Zhang Shaojun Liu Qian Liu Songqiang Zhu Xiaodong Li Jianhua Yan Zhifu Qi Hao Bin wu State Key Laboratory of Clean Energy Utilization Zhejiang UniversityHangzhou 310027ZhejiangChina Baima Lake Laboratory Hangzhou 310053ZhejiangChina Laboratory of Clean Energy and Carbon Neutrality of Zhejiang Province Jiaxing Research InstituteZhejiang UniversityJiaxing 314031ZhejiangChina Key Lab of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina Institute for Composites Science Innovation(InCSI)and State Key Laboratory of Silicon Materials School of Materials Science and EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina

The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH_(3) synthesis.In this study,we reveal that the hybrid Cu^(+)/Cu~0 interface is catalytically active for electrochemical ammonia synthesis from nitrate reduction.To maintain the hybrid Cu^(+)/Cu~0 state at negative reaction potentials,hydrophilic zeolite is used to modify Cu/Cu_(2)O electrocatalyst,which demonstrates an impressive NH_(3) production rate of 41.65 mg h^(-1) cm^(-2)with ~100% Faradaic efficiency of ammonia synthesis at-0.6 V vs.RHE.In-situ Raman spectroscopy unveil the high activity originates from the zeolite reconstruction at the electrode–electrolyte interface,which protects the valence state of Cu~0/Cu^(+) site under negative potential and promotes electrochemical activity towards NH_(3) synthesis.

关键词： Electrochemical nitrate reduction reaction Ammonia synthesis In-situ Raman spectroscopy Zeolite Density functional theory

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Review of low-temperature plasma nitrogen fixation technology

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Waste Disposal and Sustainable Energy 2021年第3期3卷 201-217页

作者： Hang Chen Dingkun Yuan angjian wu Xiaoqing Lin Xiaodong Li State Key Laboratory of Clean Energy Utilization Department of Energy EngineeringZhejiang UniversityHangzhou 310027China College of Metrology and Measurement Engineering China Jiliang UniversityHangzhou 310018China

Nitrogen fixation is essential for all forms of life,as nitrogen is required to biosynthesize fundamental building blocks of creatures,plants,and other life forms.As the main method of artificial nitrogen fixation,Haber–Bosch process(ammonia synthesis)has been supporting the agriculture and chemical industries since the 1910s.However,the disadvantages inherent to the Haber–Bosch process,such as high energy consumption and high emissions,cannot be ignored.Therefore,developing a green nitrogen fixation process has always been a research hotspot.Among the various technologies,plasma-assisted nitrogen fixation technology is very promising due to its small scale,mild reaction conditions,and flexible parameters.In the present work,the basic principles of plasma nitrogen fixation technology and its associated research progress are reviewed.The production efficiency of various plasmas is summarized and compared.Eventually,the prospect of nitrogen fixation using low-temperature plasma in the future was proposed.

关键词： Plasma Ammonia synthesis Nitrogen oxides Plasma activated water

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Waste Disposal and Sustainable Energy 2020年第2期2卷 81-84页

作者： Yufeng Ma Xiaoqing Lin angjian wu Qunxing Huang Xiaodong Li Jianhua Yan State Key Laboratory for Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou 310027China

During the period of COVID-19,the medical waste disposal capacity is seriously inadequate.The main technical process of the municipal solid waste incineration system is the same as that of the medical waste incineration system.Under the conditions of optimizing the technological process,improving the supporting facilities,and controlling the co-processing ratio,the municipal solid waste incinerator(grate furnace)co-processing medical waste is feasible.Some suggested guidelines for emergency treatment of medical waste from COVID-19 have been provided by China.

关键词： Medical waste COVID-19 Emergency treatment

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Progress in fundamental research on thermal desorption remediation of organic compound-contaminated soil

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Waste Disposal and Sustainable Energy 2021年第2期3卷 83-95页

作者： Bo Wang angjian wu Xiaodong Li Longjie Ji Chen Sun Zongze Shen Tong Chen Zuohe Chi State Key Laboratory of Clean Energy Utilization Institute of Thermal Power EngineeringZhejiang UniversityHangzhou 310027ZhejiangChina National Engineering Laboratory for Site Remediation Technologies Beijing Construction Engineering Group Environmental Remediation Co.LtdBeijing 100015China College of Metrology and Measurement Engineering China Jiliang UniversityHangzhou 310018ZhejiangChina

Thermal desorption(TD)is a mainstream technology for the remediation of organic compound-contaminated soil.By reviewing the domestic and foreign research on the remediation of organic compound-contaminated soil by TD,this paper systematically introduces the principle,characteristics,and classification of TD.The impact of key operating parameters(such as heating temperature and heating time),certain physical and chemical properties(such as soil texture,moisture content),and external conditions(such as additives and the carrier gas)on the TD process is summarized.Next,pollutants’migration and their transformation processes,as well as the laws governing the TD process,are briefly described.Finally,the prospects of TD,in terms of its future research and development directions,are described,with the aim of providing references for the application and promotion of TD.

关键词： Organic compound-contaminated soil Soil remediation Thermal desorption Fundamental research

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Ar-plasma enhanced copper-nickel alloy catalysis for ammonia synthesis

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Waste Disposal and Sustainable Energy 2022年第2期4卷 149-155页

作者： Zhou Yimeng Lv Jiabao Peng Yaqi Lin Xiaoqing Lv Xingjie Ye Qiulin Liu Shaojun wu angjian Li Xiaodong State Key Laboratory of Clean Energy Utilization Department of Energy EngineeringZhejiang UniversityHangzhou310028China

Ammonia(NH_(3))synthesis via electrocatalytic nitrogen reduction generally suffers from low NH_(3)yield and faradaic efficiency.Compared with activating stable,low-solubility N_(2),the electrochemical conversion of nitrates to ammonia provides a more reasonable route for NH_(3)production.Herein,we introduce Ar-plasma to enhance the interaction between copper-nickel alloys and carbon substrate to improve the performance of NH_(3)production.The NH_(3)faradaic efficiency from nitrate is nearly 100%and the yield rate is over 6000μgNH_(3)cm^(−2)h^(−1).DFT(density functional theory)calculation reveals the high performance of Cu_(50)Ni_(50)originates from the lower energy barrier on the reaction path and the closer position to the Fermi level of the d-band center.This work offers a promising strategy for plasma-modified electrocatalyst to promote ammonia synthesis via nitrate reduction.

关键词： Ammonia synthesis Plasma modification Nitrate conversion Copper-nickel alloy

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石油烃污染的土壤间接热脱附关键影响因素研究

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工程热物理学报 2022年第9期43卷 2451-2456页

作者：王容王博陈彤吴昂键浙江大学热能工程研究所能源清洁利用国家重点实验室杭州310013

为探究不同运行工况和土壤特性等因素对石油烃(Total petroleum hydrocarbons, TPHs)污染土壤间接热脱附行为的影响,基于小型管式炉热脱附装置,以重柴油污染土壤为主要研究对象,辅以大庆实地污染土壤的验证,研究了加热温度、加热时间、... 详细信息

为探究不同运行工况和土壤特性等因素对石油烃(Total petroleum hydrocarbons, TPHs)污染土壤间接热脱附行为的影响,基于小型管式炉热脱附装置,以重柴油污染土壤为主要研究对象,辅以大庆实地污染土壤的验证,研究了加热温度、加热时间、土壤粒径、初始含水率、初始污染物浓度5个参数对TPHs污染土壤热脱附过程的影响。结果表明:加热温度是影响热脱附效率的最重要因素;加热时间一定程度上可以弥补加热温度的不足,作用大小受加热温度的影响;不同粒径的土壤具有不同的比表面积和传热传质能力,故表现出不同的吸附能力和热脱附曲线趋势;土壤初始含水率对热脱附效率的影响主要体现在前期,初始含水率过高且加热温度较高时,水分迅速蒸发导致土壤结壳,会阻塞内部污染物的扩散迁移;污染物初始浓度会影响热脱附曲线的变化,但对最终热脱附效率无明显影响。

关键词：石油烃土壤热脱附

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生活垃圾热解气化二噁英生成指示物浓度分布及关联模型研究

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环境科学学报 2023年第2期43卷 300-308页

作者：贝建业项维灿詹明秀徐旭张光学吴昂键中国计量大学计量测试工程学院杭州310018 浙江大学清洁能源利用国家重点实验室杭州310027

生活垃圾热解气化过程中二噁英在线监测关联模型缺失.本文研究了不同反应气氛、氯源条件下生活垃圾热解气化过程中二噁英及指示物氯苯、多环芳烃的排放特性,利用SPSS软件量化二噁英与前驱物氯苯、多环芳烃之间的相关性.结果表明,由于还... 详细信息

生活垃圾热解气化过程中二噁英在线监测关联模型缺失.本文研究了不同反应气氛、氯源条件下生活垃圾热解气化过程中二噁英及指示物氯苯、多环芳烃的排放特性,利用SPSS软件量化二噁英与前驱物氯苯、多环芳烃之间的相关性.结果表明,由于还原性气氛的抑制,热解气化条件下二噁英毒性当量要比氧化性条件下低60倍.此外,12种氯苯中1,2,3-TrCBZ (1,2,3-trichlorobenzene)可作为城市生活垃圾热解气化烟气中二噁英含量的优选指示物,并建立了气相PCDD/Fs (Polychlorinated dibenzo-p-dioxins and polychlorinated dibenzofurans)与1,2,3-TrCBZ浓度的线性相关模型.16种多环芳烃中BKF(苯并荧蒽)和DbA (二苯并蒽)与二噁英总量、毒性当量的关联性一般,R2在0.7左右.本研究可为热解气化条件下二噁英在线监测关联模型的建立提供理论指导.

关键词：生活垃圾热解气化二噁英指示物关联模型

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Co-synthesis of vertical graphene nanosheets and high-value gases using inductively coupled plasma enhanced chemical vapor deposition

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Plasma Science and Technology 2018年第12期20卷 86-95页

作者：杨健许睿飏吴昂键李晓东李澧沈望俊严建华 State Key Laboratory of Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou 310027People's Republic of China Department of Nuclear Engineering University of California at BerkeleyBerkeleyCalifornia 94720United States of America China United Engineering Corporation Hangzhou 310052People's Republic of China

One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties of the ICPECVD process were revealed via electrical diagnosis and optical emission spectroscopy. The coil current and voltage increased linearly with the augmenting of injected power, and CH, C2, H2 and H were detected at a wavelength from 300 to 700 nm, implying the generation of abundant graphene-building species. The morphology and structure of solid carbon products, graphene nanosheets, were systemically characterized in terms of the variations of operating conditions, such as pressure, temperature, gas proportion, etc. The results indicated that an appropriate operating condition was indispensable for the growth process of graphene nanosheets. In the present work, the optimized result was achieved at the pressure, heating temperature, applied power and gas proportion of 600 mTorr, 800 ~C, 500 W and 20：20：15, respectively, and the augmenting of both CH4 and H2 concentrations had a positive effect on the etching of amorphous carbon. Additionally, H2 and C2 hydrocarbons were detected as the main exhaust gases. The selectivity of H2 and C2H2, measured in exhaust gases, reached up to 52% and 8%, respectively, which implied a process of free radical reactions and electron collision dissociation. Based on a comprehensive investigation of spectral and electrical parameters and synthesized products, the reaction mechanism of collision, dissociation, diffusion, etc, in ICPECVD could be speculated, providing a probable guide for experimental and industrial applications.

关键词： vertical graphene nanosheets gaseous products OES electrical diagnosis ICPECVD

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