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CuPc/FeNC双组分催化剂协同催化硝酸盐转化为氨
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作者 王毅 王硕 +6 位作者 付云凡 桑佳琪 臧一鹏 魏鹏飞 李合肥 汪国雄 包信和 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第1期104-113,共10页
氨(NH_(3))作为重要的化学品和能源储存介质,需求量与日俱增.本文旨在通过电化学硝酸根还原反应(NO_(3)^(−)RR),将NO_(3)^(−)转化为NH3,不仅解决了NO_(3)^(−)引起的环境污染问题,又可以满足对NH_(3)的迫切需求.然而,NO_(3)^(−)RR涉及多... 氨(NH_(3))作为重要的化学品和能源储存介质,需求量与日俱增.本文旨在通过电化学硝酸根还原反应(NO_(3)^(−)RR),将NO_(3)^(−)转化为NH3,不仅解决了NO_(3)^(−)引起的环境污染问题,又可以满足对NH_(3)的迫切需求.然而,NO_(3)^(−)RR涉及多个电子和质子转移过程,其中,NO_(2)^(−)是NO_(3)^(−)活化转化和深度还原合成NH_(3)的重要中间体.酞菁铜(CuPc)能够高效地活化转化NO_(3)^(−)为NO_(2)^(−),但在低过电位时无法有效地将NO2−还原为NH3,难以获得较高的氨法拉第效率(FENH3)和分电流密度.而氮配位的铁单原子催化剂(FeNC)则有较好的NO_(2)^(−)吸附活化特性.因此,利用双组分催化剂之间的协同作用以实现高效NO_(3)^(−)RR的活性和选择性是本文的主要研究思路.本文设计了CuPc/FeNC串联催化剂,利用CuPc和FeNC对NO_(3)^(−)和NO_(2)^(−)的吸附活化能力的差异,实现了高效的协同催化转化.X射线衍射、高角环形暗场扫描透射电镜、X射线光电子能谱及X射线吸收谱结果表明,FeNC催化剂中Fe原子均匀分布于ZIF-8热解后的基底.通过将FeNC和CuPc负载于气体扩散电极,在流动电解池中完成NO_(3)^(−)RR.CuPc/FeNC催化剂在较低电势区间中能够实现接近100%的NH3法拉第效率,同时在−0.57 V vs.RHE时达到273 mA cm–2的NH3分电流密度,并且在整个电势范围内有效地抑制了NO_(2)^(–)聚集.与单组分催化剂CuPc和FeNC对比结果表明,在−0.53 V vs.RHE时,CuPc/FeNC催化剂表现出较高的FE(NH_(3))/FE(NO_(2)^(−))比值,是CuPc催化剂的50倍;同时CuPc/FeNC催化剂上NH3分电流密度是FeNC催化剂的1.5倍.进一步研究了NO_(3)^(–)RR中的串联反应机制,其中FeNC催化剂表现出较高的NO_(2)^(–)RR活性,并且有效抑制了析氢反应.此外,CuPc/FeNC催化剂和FeNC催化剂在NO_(2)^(−)RR中表现出类似的NH3分电流密度,这表明在NO_(3)^(−)RR中,CuPc/FeNC催化剂性能的提高来源于FeNC位点能够进一步还原CuPc位点产生的NO_(2)^(–).理论计算结果表明,FeNC比CuPc表现出更强的NO_(2)^(–)吸附活化能力,说明NO_(2)^(−)在FeNC上更容易进行加氢还原.NO_(3)^(−)RR反应全路径分析结果表明,对于^(*)NO_(3)还原到*NO2过程,CuPc相对于FeNC位点具有明显降低的反应自由能,说明CuPc有利于NO_(2)^(−)的生成;而FeNC位点在后续的^(*)NO_(2)还原合成^(*)NH_(3)过程中具有更低的反应自由能,这与实验结果一致.一系列非原位和原位表征证明了CuPc催化剂在高电位下存在少量金属颗粒析出,与CuPc催化剂在高电位下NH_(3)分电流密度快速增加结果一致.综上,本工作中CuPc和FeNC催化剂之间的协同作用弥补了各自的不足,通过串联反应机制,在低过电位下有效增加了NH_(3)的法拉第效率和电流密度,实现了高效的协同催化转化,为设计和合成高效催化剂提供了新思路. 展开更多
关键词 硝酸根电化学还原为氨 协同催化转化 串联催化 双组分催化剂 动态现场原位表征
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Amorphous Sn(HPO_(4))_(2)-derived phosphorus-modified Sn/SnO_(x) core/shell catalyst for efficient CO_(2) electroreduction to formate
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作者 Chunfeng Cheng Tianfu Liu +7 位作者 Yi wang Pengfei Wei Jiaqi Sang Jiaqi Shao Yanpeng Song Yipeng Zang Dunfeng Gao guoxiong wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第6期125-131,I0005,共8页
Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,deriv... Simultaneously achieving high activity,selectivity and stability for electrochemical CO_(2)reduction reaction(CO_(2)RR)remains great challenges.Herein,a phosphorus-modified Sn/Sn Oxcore/shell(P-Sn/SnO_x)catalyst,derived from in situ electrochemical reduction of an amorphous Sn(HPO_(4))_(2) pre-catalyst,exhibits high CO_(2)RR performance.The total Faradaic efficiency(FE)of C_(1) products is close to 100%in a broad potential range from-0.49 to-1.02 V vs.reversible hydrogen electrode,and a total current density of 315.0 m A cm^(-2)is achieved.Moreover,the P-Sn/SnO_(x) catalyst maintains a formate FE of~90%for 120 h.Density functional theory calculations suggest that the phosphorus-modified Sn/SnO_(x) core/shell structure effectively facilitates formate production by enhancing CO_(2)adsorption and improving free energy profile of formate formation. 展开更多
关键词 CO_(2)electroreduction Structural evolution Reaction intermediate Phosphorus modification Stability
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High-throughput mechanistic study of highly selective hydrogen-bonded organic frameworks for electrochemical nitrate reduction to ammonia
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作者 Shuo wang Yi wang +2 位作者 Yunfan Fu Tianfu Liu guoxiong wang 《Journal of Energy Chemistry》 SCIE EI CSCD 2023年第12期408-415,I0011,共9页
Hydrogen-bonded organic frameworks(HOFs),an emerging porous macrocyclic materials linked by hydrogen-bond,hold potential for gas separation and storage,sensors,optical,and electrocatalysts.Here,HOF-based electrocataly... Hydrogen-bonded organic frameworks(HOFs),an emerging porous macrocyclic materials linked by hydrogen-bond,hold potential for gas separation and storage,sensors,optical,and electrocatalysts.Here,HOF-based electrocatalysts are rationally developed for nitrates reduction to ammonia,allowing not only to regulate wastewater pollution but also to accomplish carbon-neutral ammonia(NH_(3))synthesis.We preform high-throughput computational screening of thirty-six HOFs with various metals as active sites,denoted as HOF-M1,for nitrate reduction reaction(NO_(3)RR)toward NH_(3).We have implemented a hierarchical four-step screening strategy,and ultimately,HOF-Ti1 was selected based on its exceptional catalytic activity and selectivity in the NO_(3)RR process.Through additional analysis,we discovered that the d band center of the active metal sites serves as an effective parameter for designing and predicting the performance of HOFs in NO_(3)RR.This research not only showcases the immense potential of electrocatalysis in transforming NO_(3)RR into NH_(3)but also provides researchers with a compelling incentive to undertake further experimental investigations. 展开更多
关键词 Nitrate reduction reaction Ammonia synthesis Hydrogen-bonded organic frameworks High-throughput calculations ELECTROCATALYSTS
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能源催化材料的电化学合成 被引量:5
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作者 高敦峰 李合肥 +3 位作者 魏鹏飞 王毅 汪国雄 包信和 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第4期1001-1016,共16页
电催化是发展可持续洁净能源技术的基础科学,是电化学能源转换和物质转化的关键环节.精准合成催化活性纳米结构是制约很多电催化反应走向实际应用的重要挑战.与湿化学合成、固相合成和气相沉积等传统方法相比,电化学合成是一种简单、快... 电催化是发展可持续洁净能源技术的基础科学,是电化学能源转换和物质转化的关键环节.精准合成催化活性纳米结构是制约很多电催化反应走向实际应用的重要挑战.与湿化学合成、固相合成和气相沉积等传统方法相比,电化学合成是一种简单、快速、廉价及可控的高效催化材料制备方法,也是一种最为直接的一体化电极制备方法.本文综述了近年来利用电化学合成方法制备高效能源催化材料的研究进展.首先,简要介绍了电沉积、阴极腐蚀、电化学去合金化、电化学置换、电化学剥离和电化学修饰等几种主要电化学合成方法的基本原理,并讨论了电化学合成中电势、电流和电解质组成等关键合成参数的影响.然后,重点讨论了电化学合成的催化材料在燃料电池、电解水、二氧化碳/一氧化碳电还原、电化学合成氨、有机分子电化学转化等重要电催化反应中的应用.这些催化材料按照形貌可分为单原子催化剂、球形纳米粒子、形貌可控的纳米粒子、二维层状/片状纳米材料和三维纳米结构等.电化学合成在制备结构明确的单原子催化剂上具有其它合成方法不可比拟的优势.与胶体化学方法相比,电化学合成的尺寸和形貌可控的纳米粒子具有表面清洁、无表面附着的有机配体以及不需要焙烧等催化剂预处理的特点.除形貌外,电化学合成还可以制备在原子尺度上具有特定几何和电子结构的催化活性纳米结构.电化学方法也是催化剂修饰和再生的一种重要途径,结合特定的电化学程序,可在连续操作条件下实现催化材料的原位再生.通过讨论代表性的催化剂案例,分析这些催化剂在电催化应用中的构效关系,阐明了电化学合成方法在催化剂理性设计和制备中的独特优势.最后,总结了当前电化学合成催化材料方面存在的问题和研究挑战,并展望了未来的发展方向.电化学合成的能源催化材料在热催化、光催化等领域的应用价值仍需进一步探索.此外,电化学合成在金属有机框架、高熵合金等新兴功能材料的制备上也具有很好的应用前景.如何利用电化学的特点并结合原位表征、大数据预测等先进实验和理论方法,更加精准、可控地合成催化活性纳米结构依然是未来该领域重要的研究机遇. 展开更多
关键词 催化材料 电化学合成 电催化反应 电沉积 阴极腐蚀 纳米结构
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用于二氧化碳电催化还原的电解器研究进展 被引量:6
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作者 高敦峰 魏鹏飞 +3 位作者 李合肥 林龙 汪国雄 包信和 《物理化学学报》 SCIE CAS CSCD 北大核心 2021年第5期118-132,共15页
可再生能源驱动的二氧化碳电催化还原反应(CO_(2)RR)是实现CO_(2)高效转化和利用的有效途径。电解器的理性设计对于提高CO_(2)RR性能及其工业放大应用具有重要意义。电解器构型及其操作条件在很大程度上决定了电极附近的局部反应环境,... 可再生能源驱动的二氧化碳电催化还原反应(CO_(2)RR)是实现CO_(2)高效转化和利用的有效途径。电解器的理性设计对于提高CO_(2)RR性能及其工业放大应用具有重要意义。电解器构型及其操作条件在很大程度上决定了电极附近的局部反应环境,从而调变催化性能。本文深度剖析了三种CO_(2)电解器(H型电解池、流动电解池和膜电极电解池)的研究进展和现状,结合文献报道,在电流密度、法拉第效率、能量效率和稳定性等四个关键性能参数上比较和讨论了不同电解器构型的优缺点及其对CO_(2)RR性能的影响。面向实际应用的CO_(2)RR研究应该把工业级电流密度作为提高其它三个指标的前提。尽管目前还存在一些问题和挑战,膜电极电解器被认为是最具工业应用前景的技术方案。本文最后提出了一些可能的研究策略和机遇,展望了该领域的未来发展趋势。 展开更多
关键词 CO_(2)电解器 电催化还原 能量效率 工业级电流密度 流动池 膜电极
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过渡金属-氮活性位点在二氧化碳电化学还原反应中的应用(英文) 被引量:4
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作者 阎程程 林龙 +1 位作者 汪国雄 包信和 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2019年第1期23-37,共15页
大气中过高的CO_2浓度严重影响自然界的碳循环平衡,对全球气候和生态环境提出了严峻挑战.但同时CO_2作为一种潜在的碳资源,可通过催化转化生成高附加值的化学品. CO_2电化学还原反应(CO_2RR)可利用太阳能、风能等可再生能源产生的电能将... 大气中过高的CO_2浓度严重影响自然界的碳循环平衡,对全球气候和生态环境提出了严峻挑战.但同时CO_2作为一种潜在的碳资源,可通过催化转化生成高附加值的化学品. CO_2电化学还原反应(CO_2RR)可利用太阳能、风能等可再生能源产生的电能将CO_2直接转化生成高附加值化学品和燃料,有助于构建'碳中性'的能源循环利用网络,具有极具潜力的应用前景.然而,活化稳定的CO_2分子需克服一定的过电势,且由于反应在水相中进行, CO_2RR与析氢反应互相竞争,因此开发高效、廉价、稳定的催化剂一直是CO_2RR研究的难点.研究表明,含有金属-氮(M-Nx)活性位的催化材料如卟啉、酞菁等大环配合物、金属有机骨架材料以及通过热解法制备的金属-氮-碳(M-N-C)材料具有优异的CO_2RR性能.本文从实验和理论两方面综述了近年来该类材料领域的相关进展,重点介绍了金属位点种类、配体结构、载体选择对催化剂本征活性的影响,并讨论了反应条件优化对CO_2RR性能提升的作用.结合原位表征和理论计算结果探讨了含M-Nx材料反应条件下活性位的结构及反应路径,为合理设计和优化CO_2RR催化剂体系提供了新思路. 展开更多
关键词 二氧化碳电化学还原反应 金属-氮位点 含金属-氮位点的大环化合物 金属有机骨架 沸石咪唑骨架 金属-氮掺杂碳材料
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Improving the performance of solid oxide electrolysis cell with gold nanoparticles-modified LSM-YSZ anode 被引量:5
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作者 Yuefeng Song Xiaomin Zhang +5 位作者 Yingjie Zhou Houfu Lv Qingxue Liu Weicheng Feng guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第8期181-187,I0007,共8页
Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto con... Gold, as the common current collector in solid oxide electrolysis cell(SOEC), is traditionally considered to be inert for oxygen evolution reaction at the anode of SOEC. Herein, gold nanoparticles were loaded onto conventional strontium doped lanthanum manganite-yttria stabilized zirconia(LSM-YSZ) anode, which evidently improved the performance of oxygen evolution reaction at 800 °C. The current densities at 1.2 V and 1.4 V increased by 60.0% and 46.9%, respectively, after loading gold nanoparticles onto the LSM-YSZ anode. Physicochemical characterizations and electrochemical measurements suggested that the improved SOEC performance was attributed to the accelerated electron transfer of elementary process in anodic polarization reaction and the newly generated triple phase boundaries in gold nanoparticles-loaded LSMYSZ anode. 展开更多
关键词 Solid oxide ELECTROLYSIS cell Oxygen evolution reaction Gold nanoparticles CO2 ELECTROLYSIS STRONTIUM doped LANTHANUM manganite-yttria stabilized zirconia
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Co-electrolysis of CO_2 and H_2O in high-temperature solid oxide electrolysis cells: Recent advance in cathodes 被引量:7
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作者 Xiaomin Zhang Yuefeng Song +1 位作者 guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第5期839-853,共15页
Co-electrolysis of CO2and H2O using high-temperature solid oxide electrolysis cells(SOECs) into valuable chemicals has attracted great attentions recently due to the high conversion and energy efficiency,which provide... Co-electrolysis of CO2and H2O using high-temperature solid oxide electrolysis cells(SOECs) into valuable chemicals has attracted great attentions recently due to the high conversion and energy efficiency,which provides opportunities of reducing CO2emission, mitigating global warming and storing intermittent renewable energies. A single SOEC typically consists of an ion conducting electrolyte, an anode and a cathode where the co-electrolysis reaction takes place. The high operating temperature and difficult activated carbon-oxygen double-bond of CO2put forward strict requirements for SOEC cathode. Great efforts are being devoted to develop suitable cathode materials with high catalytic activity and excellent long-term stability for CO2/H2O electro-reduction. The so far cathode material development is the key point of this review and alternative strategies of high-performance cathode material preparation is proposed. Understanding the mechanism of CO2/H2O electro-reduction is beneficial to highly active cathode design and optimization. Thus the possible reaction mechanism is also discussed. Especially, a method in combination with electrochemical impedance spectroscopy(EIS) measurement, distribution functions of relaxation times(DRT) calculation, complex nonlinear least square(CNLS) fitting and operando ambient pressure X-ray photoelectron spectroscopy(APXPS) characterization is introduced to correctly disclose the reaction mechanism of CO2/H2O co-electrolysis. Finally, different reaction modes of the CO2/H2O coelectrolysis in SOECs are summarized to offer new strategies to enhance the CO2conversion. Otherwise,developing SOECs operating at 300-600 °C can integrate the electrochemical reduction and the Fischer-Tropsch reaction to convert the CO2/H2O into more valuable chemicals, which will be a new research direction in the future. 展开更多
关键词 SOECs Co-electrolysis Carbon dioxide STEAM CATHODE
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Infiltration of Ce0.8Gd0.2O1.9 nanoparticles on Sr2Fe1.5Mo0.5O6-δ cathode for CO2 electroreduction in solid oxide electrolysis cell 被引量:5
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作者 Houfu Lv Yingjie Zhou +4 位作者 Xiaomin Zhang Yuefeng Song Qingxue Liu guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2019年第8期71-78,I0004,共9页
Solid oxide electrolysis cell(SOEC) can electrochemically convert CO2 to CO at the gas-solid interface with a high current density and Faradaic efficiency, which has attracted increasing attentions in recent years.Exp... Solid oxide electrolysis cell(SOEC) can electrochemically convert CO2 to CO at the gas-solid interface with a high current density and Faradaic efficiency, which has attracted increasing attentions in recent years.Exploring efficient catalyst for electrochemical CO2 reduction reaction(CO2 RR) at the cathode is a grand challenge for the research and development of SOEC. Sr2Fe1.5Mo0.5O6-δ(SFM) is one kind of promising cathode materials for SOEC, but suffers from insufficient activity for CO2 RR. Herein, Gd0.2Ce0.8O1.9(GDC)nanoparticles were infiltrated onto the SFM surface to construct a composite GDC-SFM cathode and improve the CO2 RR performance in SOEC. The current density over the GDC infiltrated SFM cathode with a GDC loading of 12.8 wt% reaches 0.446 A cm-2 at 1.6 V and 800 °C, which is much higher than that over the SFM cathode(0.283 A cm-2). Temperature-programmed desorption of CO2 measurements suggest that the infiltration of GDC nanoparticles significantly increases the density of surface active sites and three phase boundaries(TPBs), which are beneficial for CO2 adsorption and subsequent conversion. Electrochemical impedance spectroscopy results indicate that the polarization resistance of 12.8 wt% GDCSFM cathode was obviously decreased from 0.46 to 0.30 cm^2 after the infiltration of GDC nanoparticles. 展开更多
关键词 Electrochemical carbon dioxide reduction reaction Solid oxide ELECTROLYSIS cell Double PEROVSKITE INFILTRATION
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Nitrogen-doped carbon nanotube encapsulating cobalt nanoparticles towards efficient oxygen reduction for zinc–air battery 被引量:4
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作者 Haihua Wu Xiaole Jiang +5 位作者 Yifan Ye Chengcheng Yan Songhai Xie Shu Miao guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第6期1181-1186,共6页
Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt s... Nitrogen-doped carbon materials encapsulating 3 d transition metals are promising alternatives to replace noble metal Pt catalysts for efficiently catalyzing the oxygen reduction reaction(ORR). Herein, we use cobalt substituted perfluorosulfonic acid/polytetrafluoroethylene copolymer and dicyandiamide as the pyrolysis precursor to synthesize nitrogen-doped carbon nanotube(N–CNT) encapsulating cobalt nanoparticles hybrid material. The carbon layers and specific surface area of N–CNT have a critical role to the ORR performance due to the exposed active sites, determined by the mass ratio of the two precursors. The optimum hybrid material exhibits high ORR activity and stability, as well as excellent performance and durability in zinc–air battery. 展开更多
关键词 Nitrogen-doped carbon nanotube Perfluorosulfonic Acid/polytetrafluoroethylene copolymer Cobalt substitution Oxygen reduction reaction Zinc–air battery
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Gas-phase electrocatalytic reduction of carbon dioxide using electrolytic cell based on phosphoric acid-doped polybenzimidazole membrane 被引量:3
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作者 Dunfeng Gao Fan Cai +3 位作者 Qinqin Xu guoxiong wang Xiulian Pan Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2014年第6期694-700,共7页
Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an el... Carbon dioxide transformation to fuels or chemicals provides an attractive approach for its utilization as feedstock and its emission reduction. Herein, we report a gas-phase electrocatalytic reduction of CO2 in an electrolytic cell, constructed using phosphoric acid-doped polybenz- imidazole (PBI) membrane, which allowed operation at 170 ℃ Pt/C and PtMo/C with variable ratio of Pt/Mo were studied as the cathode catalysts. The results showed that PtMo/C catalysts significantly enhanced CO formation and inhibited CH4 formation compared with Pt/C catalyst. Characterization by X-ray diffraction, X-ray photoelectron spectroscopy and transmission electron microscopy revealed that most Mo species existed as MoO3 in PtMo/C catalysts and the interaction between Pt and MoOx was likely responsible for the enhanced CO formation rate although these bicomponent catalysts in general had a larger particle size than Pt/C catalyst. 展开更多
关键词 carbon dioxide gas-phase electrocatalytic reduction platinum-molybdenum catalyst Faradaic efficiency formation rate
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Two-step pyrolysis of ZIF-8 functionalized with ammonium ferric citrate for efficient oxygen reduction reaction 被引量:3
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作者 Yifan Ye Fan Cai +3 位作者 Chengcheng Yan Yanshuo Li guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2017年第6期1174-1180,共7页
Zeolitic imidazolate frameworks(ZIFs) are widely employed in catalyst synthesis as parental materials for electrochemical energy storage and conversion. Herein, we have demonstrated a facile synthesis of highly effi... Zeolitic imidazolate frameworks(ZIFs) are widely employed in catalyst synthesis as parental materials for electrochemical energy storage and conversion. Herein, we have demonstrated a facile synthesis of highly efficient catalyst for oxygen reduction reaction in both alkaline and acidic medium, which is derived from ZIF-8 functionalized with ammonium ferric citrate via two-step pyrolysis in Ar and NHatmosphere.The results reveal that the catalytic activity improvement after NH3 pyrolysis benefits from mesoporedominated morphology and high utilization of Fe-containing active sites. The optimum catalyst shows excellent performance in zinc-air battery and polymer electrolyte membrane fuel cell tests. 展开更多
关键词 Zeolitic imidazolate frameworks Two-step pyrolysis Oxygen reduction reaction Zinc-air battery Polymer electrolyte membrane fuel cell
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Doped all-inorganic cesium zirconium halide perovskites with high-efficiency and tunable emission 被引量:2
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作者 Pengfei Cheng Daoyuan Zheng +6 位作者 Lu Feng Yuefeng Liu Junxue Liu Juntao Li Yang Yang guoxiong wang Keli Han 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2022年第2期600-604,共5页
Doping enables manipulation of both the electrical and optical properties of halide perovskites.Herein,we incorporated Te^(4+) into Cs_(2)ZrCl_(6) single crystal,simultaneously preserving the vacancy-ordered structure... Doping enables manipulation of both the electrical and optical properties of halide perovskites.Herein,we incorporated Te^(4+) into Cs_(2)ZrCl_(6) single crystal,simultaneously preserving the vacancy-ordered structure,to obtain an efficient yellow-emitting perovskite with a near-unity photoluminescence quantum yield(PLQY≈97.6%).Te^(4+) doping modifies the hue and emission color of pristine Cs_(2)ZrCl_(6),generates new absorption channels,and successfully extends the excitation energy from<280 nm to 360-450 nm range.Detailed spectral characterizations,including ultrafast femtosecond transient absorption measurements,reveal that the bright yellow light is derived from triplet self-trapped excitons.Moreover,further tuning doping concentration enables Te-doped Cs_(2)ZrCl_(6) single crystals to exhibit efficient warm white light emission.This work provides a new perspective for the development and design of stable lead-free perovskites with highly efficient luminescence. 展开更多
关键词 Zirconium halide perovskite Doping Excitation energy Photoluminescence Energy transfer
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Heterogeneous Catalysis for CO_(2) Conversion into Chemicals and Fuels 被引量:2
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作者 Dunfeng Gao Wanjun Li +2 位作者 Hanyu wang guoxiong wang Rui Cai 《Transactions of Tianjin University》 EI CAS 2022年第4期245-264,共20页
Catalytic conversion of CO_(2)into chemicals and fuels is a viable method to reduce carbon emissions and achieve carbon neutrality.Through thermal catalysis,electrocatalysis,and photo(electro)catalysis,CO_(2)can be co... Catalytic conversion of CO_(2)into chemicals and fuels is a viable method to reduce carbon emissions and achieve carbon neutrality.Through thermal catalysis,electrocatalysis,and photo(electro)catalysis,CO_(2)can be converted into a wide range of valuable products,including CO,formic acid,methanol,methane,ethanol,acetic acid,propanol,light olefi ns,aromatics,and gasoline,as well as fi ne chemicals.In this mini-review,we summarize the recent progress in heterogeneous catalysis for CO_(2)conversion into chemicals and fuels and highlight some representative studies of diff erent conversion routes.The structure-performance correlations of typical catalytic materials used for the CO_(2)conversion reactions have been revealed by combining advanced in situ/operando spectroscopy and microscopy characterizations and density functional theory cal-culations.Catalytic selectivity toward a single CO_(2)reduction product/fraction should be further improved at an industrially relevant CO_(2)conversion rate with considerable stability in the future. 展开更多
关键词 CO_(2)conversion CO_(2)hydrogenation CO_(2)electroreduction CHEMICALS Fuels
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Preface to special column on catalytic conversion of CO_(2) 被引量:1
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作者 Yanqiang Huang Da-Gang Yu guoxiong wang 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2022年第7期1545-1546,共2页
With the increasing awareness of sustainable chemistry and green chemistry,catalytic conversion of carbon dioxide(CO_(2))into high value‐added and bulk chemicals is a promising tech‐nology that can utilize CO_(2) as... With the increasing awareness of sustainable chemistry and green chemistry,catalytic conversion of carbon dioxide(CO_(2))into high value‐added and bulk chemicals is a promising tech‐nology that can utilize CO_(2) as an ideal C1 source while simulta‐neously storing renewable energy.Despite being frustrated with its thermodynamic stability and kinetic inertness,CO_(2) has been tamed for triggering catalytic constructions of highly‐valued entities like important hydrocarbon fuels and fine chemicals,mainly aiding by two scenarios:CO_(2) reduction and CO_(2)‐involved organic synthesis.Accordingly,science,industry and govern‐ment agencies have been devoted to leverage these synthetic tools in targeting the catalytic conversion of CO_(2).Therefore,it motivates us to organize the special column of“Catalytic Con‐version of CO_(2)”.The column contains 14 papers,including 4 reviews,4 communications and 6 articles,which cover the frontiers and most of the research aspects of catalytic con‐version of CO_(2). 展开更多
关键词 CATALYTIC utilize VALUED
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Ball-milling MoS_2/carbon black hybrid material for catalyzing hydrogen evolution reaction in acidic medium 被引量:1
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作者 Jiayuan Li Dunfeng Gao +3 位作者 Jing wang Shu Miao guoxiong wang Xinhe Bao 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2015年第5期608-613,共6页
Replacing platinum for catalyzing hydrogen evolution reaction (HER) in acidic medium remains great chal- lenges. Herein, we prepared few-layered MoS2 by ball milling as an efficient catalyst for HER in acidic medium... Replacing platinum for catalyzing hydrogen evolution reaction (HER) in acidic medium remains great chal- lenges. Herein, we prepared few-layered MoS2 by ball milling as an efficient catalyst for HER in acidic medium, The activity of as-prepared MoS2 had a strong dependence on the ball milling time, Furthermore, Ketjen Black EC 300J was added into the ball-milled MoS2 followed by a second ball milling, and the resultant MoS2/carbon black hybrid material showed a much higher HER activity than MoS2 and carbon black alone. The enhanced activity of the MoS2/carbon black hybrid material was attributed to the increased abundance of catalytic edge sites of MoS) and excellent electrical coupling to the underlving carbon network. 展开更多
关键词 Molybdenum disulfide Carbon black Hybrid material Ball milling Hydrogen evolution reaction Acidic medium
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纳米氧化铜片用于高效电化学还原一氧化氮 被引量:1
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作者 邵加奇 魏鹏飞 +6 位作者 王硕 宋延鹏 付云凡 李荣坦 张小敏 汪国雄 包信和 《Science China Materials》 SCIE EI CAS CSCD 2024年第6期1876-1881,共6页
一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生... 一氧化氮电还原反应将工业废气转化为有价值的氨,表现出极具潜力的应用前景.在本工作中,我们合成了具有高比表面积和丰富缺陷的氧化铜纳米片催化剂,在流动池中氨法拉第效率达到92.1%,在-0.2 V vs.RHE时,一氧化氮电还原电流密度和氨的生产速率分别达到1.1 A cm^(-2)和7356μmol cm^(-2)h^(-1).在电流密度超过400 m A cm-2时,氨法拉第效率在50小时保持在80%以上.准原位X射线光电子能谱和原位X射线吸收光谱结果表明氧化铜纳米片在一氧化氮电还原过程中被电化学还原成单质铜.与铜纳米颗粒相比,氧化铜纳米片展现出较高的电化学表面积和一氧化氮电还原的内在活性. 展开更多
关键词 electrocatalytic NORR ammonia synthesis ELECTRO-CATALYSIS CuO nanosheets
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Inspecting design rules of metal-nitrogen-carbon catalysts for electrochemical CO_(2)reduction reaction:From a data science perspective
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作者 Rui Ding Meng Ma +4 位作者 Yawen Chen Xuebin wang Jia Li guoxiong wang Jianguo Liu 《Nano Research》 SCIE EI CSCD 2023年第1期264-280,共17页
The development of inexpensive metal-nitrogen-carbon(M-N-C)catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR)on an industrial scale has come to a standstill.Although the number of related studies and rev... The development of inexpensive metal-nitrogen-carbon(M-N-C)catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR)on an industrial scale has come to a standstill.Although the number of related studies and reviews has grown fast,the complexity of the M-N-C composite has limited researchers to focus on only a few variables and carry out sluggish trial-and-error optimizations in their studies.As a result,the conclusions are drawn only by artificial analysis based on a few orthogonal experimental results.To obtain more general design strategies,we have innovatively introduced machine learning(ML)into this field to address this bottleneck.A standard workflow that comprehensively utilizes different ML algorithms and black-box interpretation methods is proposed for this purpose.Besides predicting CO_(2)RR performance metrics for M-N-C catalysts,such as maximum faradaic efficiency with great accuracy,the ML models have also indicated simple and clear design strategies that would guide future exploration from a data science perspective.Besides,we have also demonstrated the potential of the models in guiding the development of new material systems.We thereby believe that the new research paradigm proposed may accelerate the development of this field soon. 展开更多
关键词 electrochemical CO_(2)reduction reaction metal-nitrogen-carbon catalyst machine learning artificial intelligence data science
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调控双钙钛矿中高熵组分促进高温析氧反应
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作者 冯炜程 于景成 +8 位作者 杨溢澜 郭宜阁 邹庚 刘晓菊 陈洲 董坤 宋月锋 汪国雄 包信和 《物理化学学报》 SCIE CAS 2024年第6期41-43,共3页
固体氧化物电解池(SOEC)中阳极析氧反应动力学较为迟缓,限制了SOEC器件电催化转化能力,因此针对阳极材料的改性研究对于进一步提升SOEC电化学性能十分关键。高熵钙钛矿(HEP)在许多反应中表现出良好的催化活性,但在SOEC中的应用鲜有研究... 固体氧化物电解池(SOEC)中阳极析氧反应动力学较为迟缓,限制了SOEC器件电催化转化能力,因此针对阳极材料的改性研究对于进一步提升SOEC电化学性能十分关键。高熵钙钛矿(HEP)在许多反应中表现出良好的催化活性,但在SOEC中的应用鲜有研究。本文通过在双钙钛矿的A位或A'位分别掺杂不同的稀土金属、碱土金属或碱金属离子,合成了(Pr_(0.2)La_(0.2)Sm_(0.2)Nd_(0.2)Gd_(0.2))BaCo_(2)O_(6-δ)(A-HEP)和Pr(Ba_(0.2)Sr_(0.2)Ca_(0.2)Na_(0.2)K_(0.2))Co_(2)O_(6-δ)(A'-HEP)两种高熵钙钛矿材料。由于掺杂离子平均半径和氧化态的差异,A-HEP保持四方双钙钛矿相结构而A'-HEP则转变为正交单钙钛矿相。物理化学表征结果表明,A-HEP中Co平均价态更高,Co 2p-O 1s杂化更强,从而增加了电子转移路径并降低了转移能垒。同时,A-HEP中表面氧空位浓度更高,可为阳极析氧反应提供更多的活性位点。因此,在具有A-HEP阳极的SOEC中,与氧输运、电子传输和表界面反应过程相关的阳极极化电阻显著降低,并在800℃下实现最高1.76 A·cm^(-2)的电流密度和200 h的稳定性。本工作为高熵钙钛矿材料在SOEC阳极中的应用提供了新的策略。 展开更多
关键词 固体氧化物电解池 高熵钙钛矿 析氧反应 氧空位 电子转移
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基于等温吸附实验的煤层气解吸阶段数值描述 被引量:29
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作者 张政 秦勇 +1 位作者 guoxiong wang 傅雪海 《中国科学:地球科学》 CSCD 北大核心 2013年第8期1352-1358,共7页
煤层气解吸阶段的定量描述是客观认识煤层气井产能、诊断煤层气井生产状况及优化排采管理的重要基础.本文基于沁水盆地南部6口煤层气井的12件无烟煤样品进行了一系列的等温吸附实验,并以此为基础,建立了一种以朗格缪尔吸附理论为基础的... 煤层气解吸阶段的定量描述是客观认识煤层气井产能、诊断煤层气井生产状况及优化排采管理的重要基础.本文基于沁水盆地南部6口煤层气井的12件无烟煤样品进行了一系列的等温吸附实验,并以此为基础,建立了一种以朗格缪尔吸附理论为基础的解析模型.运用此模型,建立了以等效解吸率及其曲线特征来刻画煤层气解吸阶段性的数值方法.通过实验和数值描述,以等效解吸率曲率为依据,提出并确定了启动压力、过渡压力和敏感压力三个定义降压解吸阶段的关键压力点.在此基础上,将等温吸附实验下煤层气的解吸过程划分为四个阶段,即零解吸阶段、缓慢解吸阶段、过渡解吸阶段和敏感解吸阶段.通过类比分析,发现等温吸附实验条件下的煤层气解吸阶段性与煤层气井产气过程的异同之处,认为较高的朗格缪尔体积和朗格缪尔常数比有利于稳产阶段的及早到来,但也可能使煤层气产能递减阶段提前出现. 展开更多
关键词 煤层气 等温吸附 等效解吸率 关键压力 解吸阶段 数值描述
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