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Efficient nitrate electroreduction over Mn-doped Cu catalyst via regulating N-containing intermediates adsorption configuration

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Science China Chemistry 2024年第6期67卷 1969-1975页

作者： Limin Wu shunhan jia Libing Zhang Ruhan Wang jiaqi Feng Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences CAS Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing100049China College of Chemical Engineering and Environment China University of PetroleumBeijing102249China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China

The electrochemical reduction of NO_(3)^(-)to NH_(3)holds promise for economic and environmental benefits,presenting an energyefficient alternative to the traditional Haber-Bosch ***,challenges exist due to its sluggish kinetics,multiple intermediates,and various reaction *** this study,Mn-doped-Cu catalyst was synthesized and employed for electrochemical NO_(3)^(-)-to-NH_(3)*** doping of Mn into Cu resulted in exceptional performance,achieving a FE of 95.8%and an NH_(3)yield rate of 0.91 mol g^(-1)h^(-1)at-0.6 V in a neutral electrolyte at low NO_(3)^(-)*** experimental studies and theoretical calculations revealed that the Mn dopant enhanced the kinetic rate of NO_(2)~--to-NH_(3)and induced a distinct configuration of**** alteration decreased the energy barrier of*NO-to-*NOH,consequently promoting the conversion of NO_(3)^(-)-to-NH_(3).

关键词： nitrate reduction electrocatalysis ammonia synthesis N-intermediate green chemistry

Flexible and tailorable quasi‐solid‐state rechargeable Ag/Zn microbatteries with high performance

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Carbon Energy 2021年第1期3卷 167-175页

作者： Songshan Bi Fang Wan Shuai Wang shunhan jia Jinlei Tian Zhiqiang Niu Key Laboratory of Advanced Energy Materials Chemistry(Ministry of Education) College of ChemistryNankai UniversityTianjinChina

The recent boom in flexible and wearable electronics requires their powersources not only to be adequately compact but also could undergo extremedeformation without significant degradation in performance. Here, flexibleand tailorable quasi‐solid‐state microsized Ag/Zn batteries (micro‐AZBs)were designed by combining mask‐assisted spray printing and electrochemicaldeposition strategies. The micro‐AZBs display ultrastable outputvoltage, excellent energy, and power densities, as well as stable cycling ***, the micro‐AZBs with desired shapes can be designedin series or in parallel on a flexible chip to output improved voltage or currentwith the internal connection. More importantly, the microelectrodes could besprayed on various substrates. Flexible micro‐AZBs could be achieved onflexible substrates and tailorable micro‐AZBs are obtained when they arefabricated on clothes. They exhibit stable electrochemical performance evenunder bending or cutting states. The novel design of such quasi‐solid‐statemicro‐AZBs would pave a way for the miniaturization and integration ofenergy storage devices.

关键词： Ag/Zn microbattery flexibility tailorability

Multicomponent catalyst design for CO2/N2/NOx electroreduction

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Industrial Chemistry & Materials

Industrial Chemistry & Materials 2023年第1期1卷 93-105页

作者： shunhan jia Limin Wu Liang Xu Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing100190China School of Chemical Sciences University of Chinese Academy of SciencesBeijing100049China Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai200062China

Electroreduction of small molecules such as CO2,N2,and NO3−is one of the promising routes to produce sustainable chemicals and fuels and store renewable energy,which could contribute to our carbon neutrality *** multicomponent electrocatalysts,integrating the advantages of individual components of catalysts,are of great importance to achieve efficient electroreduction of small molecules via activation of inert bonds and multistep *** this review,some basic issues in the electroreduction of small molecules including CO2,N2,and NO3−are briefly *** then discuss our fundamental understanding of the rule of interaction in multicomponent electrocatalysts,and summarize three models for multicomponent catalysts,including type I,“a non-catalytically active component can activate or protect another catalytic component”;type II,“all catalytic components provide active intermediates for electrochemical conversion”;and type III,“one component provides the substrate for the other through conversion or adsorption”.Additionally,an outlook was considered to highlight the future directions of multicomponent electrocatalysts toward industrial applications.

关键词： Green chemistry Green carbon science Electroc atalysis Synergetic effect

Electrochemical Transformation of CO_(2)to Value-Added Chemicals and Fuels

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CCS Chemistry 2022年第10期4卷 3213-3229页

作者： shunhan jia Xiaodong Ma Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Colloid and Interface and ThermodynamicsCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062

CO_(2)is the main greenhouse gas and a renewable carbon *** transformation of CO_(2)(CO_(2)ET)to value-added chemicals and fuels is one of the promising routes to reduce CO_(2)emission and contributes to sustainability and carbon *** this review,we discuss recent developments on apparatuses used in CO_(2)ET,electrocatalytic reactions of CO_(2)with water,organics,nitrogen,and nitrogen-containing compounds to synthesize chemicals and fuels by the construction of different chemical bonds(e.g.,C–H,C–C,C–O,and C–N),and related reaction ***,an outlook was considered to highlight the opportunities and challenges in CO_(2)ET.

关键词： carbon dioxide green chemistry green carbon science electro-organic synthesis catalysis

Asymmetric Cu Sites for Enhanced CO_(2)Electroreduction to C_(2+)Products

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CCS Chemistry 2024年第5期6卷 1231-1239页

作者： Weiwei Guo Xingxing Tan shunhan jia Shoujie Liu Xinning Song Xiaodong Ma Limin Wu Lirong Zheng Xiaofu Sun Buxing Han Beijing National Laboratory for Molecular Sciences Key Laboratory of Colloid and Interface and ThermodynamicsCenter for Carbon Neutral ChemistryInstitute of ChemistryChinese Academy of SciencesBeijing 100190 Institute of Molecular Metrology College of Chemistry and Chemical EngineeringQingdao UniversityQingdao 266071 School of Chemical Sciences University of Chinese Academy of SciencesBeijing 100049 School of Materials Science and Engineering Anhui UniversityHefei 230601 Institute of High Energy Physics Chinese Academy of SciencesBeijing 100049 Shanghai Key Laboratory of Green Chemistry and Chemical Processes School of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062

Cu-based electrocatalysts can have excellent activity for the generation of C_(2+)products from a CO_(2)reduction reaction(CO_(2)RR).Cuδ+species is crucial in tuning the performance of the ***,we discovered that Si-doped Cu catalysts had excellent performance for electrochemical CO_(2)to C_(2+)products.A high Faradaic efficiency(FE)of 84.7%was achieved with a current density of 289mA cm^(−2)in the flow-cell *** situ experimental results showed that the significant reconstruction occurred during the electrolysis,resulting in the formation of the asymmetric Cu sites(Cu^(0)-Cu^(+)).The ratio of Cu^(0)and Cu^(+)could be tuned by changing Si *** experiments and theoretical calculations demonstrated that the asymmetric Cu sites caused by the appropriate Si doping promoted CO_(2)activation and strengthened the adsorption of^(*)CO *** was beneficial to the subsequent^(*)CO–^(*)CO dimerization step,and thus,accounted for the enhancement of C_(2+)selectivity.

关键词： carbon dioxide electrocatalysis asymmetric Cu sites C-C coupling green chemistry

CO_(2)参与电化学构筑C—N键制备重要化学品

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高等学校化学学报 2022年第7期43卷 202-212页

作者：王茹涵贾顺涵吴丽敏孙晓甫韩布兴中国科学院胶体、界面与化学热力学重点实验室中国科学院化学研究所北京100190 中国科学院大学化学科学学院北京100149 上海市绿色化学与化工过程绿色化重点实验室华东师范大学化学与分子工程学院上海200062

CO_(2)是主要的温室气体,同时也是重要的C1资源.通过构筑C—N键制备重要化学品在化工、生物合成及医药等领域应用广泛.近年来,随着碳中和与绿色化学理念的不断深化,电化学构筑C—N键的策略也因其环保、低碳、简单及绿色等优势而受到关注... 详细信息

CO_(2)是主要的温室气体,同时也是重要的C1资源.通过构筑C—N键制备重要化学品在化工、生物合成及医药等领域应用广泛.近年来,随着碳中和与绿色化学理念的不断深化,电化学构筑C—N键的策略也因其环保、低碳、简单及绿色等优势而受到关注.同时,由于化石燃料不断消耗带来的资源与环境问题,重要化学品及燃料的绿色合成也成为科技发展战略中的重中之重.本文归纳了CO_(2)参与构建C—N键制备重要化学品方面的研究进展;从催化体系构建、反应过程和机理的角度对电化学合成尿素、酰胺和胺进行了综述;最后针对目前研究中面临的挑战,对这一领域的未来发展进行了展望.

关键词： CO_(2)还原电催化 C—N耦合绿色化学

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“无中生有”的化学

大学化学 2020年第11期35卷 150-154页

作者：贾顺涵邱晓航南开大学化学学院天津300071

现代科学技术实现飞速发展,化学和以化学为中心的诸多交叉学科功不可没。本文借用成语“无中生有”,深入浅出地介绍前沿科技成果中蕴含的化学原理,帮助化学相关专业本科生理解专业课学到的理论知识,引导其关注学科发展前沿,激发其对进... 详细信息

现代科学技术实现飞速发展,化学和以化学为中心的诸多交叉学科功不可没。本文借用成语“无中生有”,深入浅出地介绍前沿科技成果中蕴含的化学原理,帮助化学相关专业本科生理解专业课学到的理论知识,引导其关注学科发展前沿,激发其对进一步了解科学研究的渴望。

关键词：化学传感器多孔材料电化学