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MoC nanocrystals confined in N-doped carbon nanosheets toward highly selective electrocatalytic nitric oxide reduction to ammonia

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Nano Research 2022年第10期15卷 8890-8896页

作者： Ge Meng Mengmeng Jin Tianran Wei Qian Liu Shusheng Zhang Xianyun Peng Jun Luo Xijun Liu Key Laboratory of Carbon Materials of Zhejiang Province College of Chemistry and Materials EngineeringWenzhou UniversityWenzhou 325035China Institute for New Energy Materials and Low-Carbon Technologies Tianjin Key Lab for Photoelectric Materials&DevicesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials and Guangxi Key Laboratory of Processing for NonFerrous Metals and Featured MaterialsSchool of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China Institute for Advanced Study Chengdu UniversityChengdu 610106China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Institute of Zhejiang University–Quzhou Quzhou 324000China

Electrochemical nitric oxide reduction reaction(NORR)to produce ammonia(NH3)under ambient conditions is a promising alternative to the energy and carbon-intensive Haber–Bosch approach,but its performance is still ***,molybdenum carbides(MoC)nanocrystals confined by nitrogen-doped carbon nanosheets are first designed as an efficient and durable electrocatalyst for catalyzing the reduction of NO to NH3 with maximal Faradaic efficiency of 89%±2%and a yield rate of 1,350±15μg·h^(−1)·cm^(−2) at the applied potential of−0.8 V *** hydrogen electrode(RHE)as well as high stable activity with negligible current density and NH3 yield rate decays over a 30 h continue the ***,as a proof-of-concept of Zn–NO battery,it achieves a peak power density of 1.8 mW·cm^(−2) and a large NH3 yield rate of 782±10μg·h^(−1)·cm^(−2),which are comparable to the best-reported *** calculations reveal that the MoC(111)has a strong electronic interaction with NO molecules and thus lowering the energy barrier of the potential-determining step and suppressing hydrogen evolution *** work suggests that Mo-based materials are a powerful platform providing great opportunities to explore highly selective and active catalysts for NH3 production.

关键词： ammonia electrosynthesis green route molybdenum carbides(MoC)nanocrystals nitric oxide reduction reaction high selectivity

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Electrocatalytic reduction of NO to NH_(3) in ionic liquids by P-doped TiO_(2) nanotubes

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Frontiers of Chemical Science and Engineering 2023年第6期17卷 726-734页

作者： Shangcong Zhang Qian Liu Xinyue Tang Zhiming Zhou Tieyan Fan Yingmin You Qingcheng Zhang Shusheng Zhang Jun Luo Xijun Liu College of Electrical and Electronic Engineering Wenzhou UniversityWenzhou 325035China Low Voltage Apparatus Technology Research Centre of Zhejiang Wenzhou UniversityWenzhou 325035China Institute for Advanced Study Chengdu UniversityChengdu 610106China College of Chemistry and Materials Engineering Wenzhou UniversityWenzhou 325035China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Tianjin Key Lab for Photoelectric Materials&Devices School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Compesite Structures School of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China

Designing advanced and cost-effective electrocatalytic system for nitric oxide(NO)reduction reaction(NORR)is vital for sustainable NH_(3) production and NO removal,yet it is a challenging ***,it is shown that phosphorus(P)-doped titania(TiO_(2))nanotubes can be adopted as highly efficient catalyst for *** catalyst demonstrates impressive performance in ionic liquid(IL)-based electrolyte with a remarkable high Faradaic efficiency of 89%and NH3 yield rate of 425μg·h^(−1)·mg_(cat).^(−1),being close to the best-reported ***,the obtained performance metrics are significantly larger than those for N_(2) reduction *** also shows good durability with negligible activity decay even after 10 *** simulations reveal that the introduction of P dopants tunes the electronic structure of Ti active sites,thereby enhancing the NO adsorption and facilitating the desorption of ^(*)NH_(3).Moreover,the utilization of IL further suppresses the competitive hydrogen evolution *** study highlights the advantage of the catalyst−electrolyte engineering strategy for producing NH_(3) at a high efficiency and rate.

关键词： nitric oxide reduction reaction electrcatalysis ammonia production phosphorus-doped titania

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Active-site and interface engineering of cathode materials for aqueous Zn–gas batteries

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Nano Research 2023年第2期16卷 2325-2346页

作者： Wenxian Liu Jinxiu Feng Tianran Wei Qian Liu Shusheng Zhang Yang Luo Jun Luo Xijun Liu College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Ministry of Education(MOE)Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourceEnvironmentsand MaterialsGuangxi UniversityNanning 530004China Institute for Advanced Study Chengdu UniversityChengdu 610106China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Empa Swiss Federal Laboratories for Materials Science and TechnologySwiss Federal Institute of Technology in Zurich(ETH)DomainDübendorf CH-8600Switzerland Hong Kong Productivity Council(HKPC) Hong Kong 999077China School of Materials Science and Engineering Tianjin University of TechnologyTianjin 300384China

Aqueous rechargeable Zn–gas batteries are regarded as promising energy storage and conversion devices due to their high safety and inherent environmental ***,the energy efficiency and power density of Zn–gas batteries are restricted by the kinetically sluggish cathode reactions,such as oxygen evolution reaction(OER)during charging and oxygen reduction reaction(ORR)/carbon dioxide reduction reaction(CO_(2)RR)/nitrogen reduction reaction(NRR)/nitric oxide reduction reaction(NORR)during *** this review,battery configurations and fundamental reactions in Zn–gas batteries are first introduced,including Zn–air,Zn-CO_(2),Zn-N_(2),and Zn-NO ***,recent advances in active site engineering for enhancing the intrinsic catalytic activities of cathode catalysts are ***,the structure and surface regulation strategies of cathode materials for optimizing the three-phase interface and improving the performance of Zn–gas batteries are ***,some personal perspectives for the future development of Zn–gas batteries are presented.

关键词： Zn–gas batteries electrocatalysis single-atom catalysts chemical doping heterostructure interface

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Study on mechanism of low-temperature oxidation of n-hexanal catalysed by 2D ultrathin Co_(3)O_(4) nanosheets

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Nano Research 2022年第2期15卷 1660-1671页

作者： Leilei Miao Xiaolong Tang Shunzheng Zhao Xizhou Xie Chengcheng Du Tian Tang Honghong Yi Department of Environmental Enginnering School of Energy and Environmental EngineeringUniversity of Science and TechnologyBeijingBeijing 100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing 100083China

Achieving high catalytic performance with lower possible cost and higher energetic efficiency is critical for catalytic oxidation of volatile organic compounds(VOCs).However,traditional thermocatalysts generally undergo low catalytic activity and fewer active ***,this paper synthesizes nearly all-surface-atomic,ultrathin two-dimensional(2D)Co_(3)O_(4) nanosheets to address these problems through offering a numerous active sites and high electron *** 2D Co_(3)O_(4) nanosheets(1.70 nm)exhibit catalyzation to the total oxidation of n-hexanal at the lower temperature of r90%=202℃,and at the space velocity of 5.0×10^(4) h^(-1).It is over 1.2 and 6 times higher catalytic activity than that of 2D CoO nanosheets(1.71 nm)and bulk Co_(3)O_(4) counterpart,*** absorption spectroscopy analysis shows that the oxygen vacancy defect traps electrons,thereby preventing the recombination with holes,increasing the lifetime of electrons,and making electron-holes reach a nondynamic *** longer the electron lifetime is,the easier the oxygen vacancy defects capture ***,the defects combine with oxygen to form active oxygen *** with the lattice oxygen involved in the reaction of bulk Co_(3)O_(4),the nanosheets change the catalytic reaction path,which effectively reduces the activation energy barrier from 34.07 to 27.15 kJ/*** changed surface disorder,the numerous coordinatively-unsaturated Co atoms and the high ratio of O_(ads)/O_(lat) on the surface of 2D Co_(3)O_(4) nanosheets are responsible for the catalytic performance.

关键词： catalytic reaction n-hexanal oxidation two-dimensional nanosheets oxygen vacancy defect coordinated unsaturated atom

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双功能Nb-N-C原子分散催化剂用于水系锌-空气电池驱动CO_(2)还原

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Science China Materials 2023年第3期66卷 1013-1023页

作者：高三双王天玮靳梦梦张书胜刘倩胡广志杨慧罗俊刘熙俊 Institute for New Energy Materials and Low-Carbon Technologies Tianjin Key Lab for Photoelectric Materials&DevicesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Institute for Advanced Study Chengdu UniversityChengdu 610106China Institute for Ecological Research and Pollution Control of Plateau Lakes School of Ecology and Environmental Science Yunnan UniversityKunming 650504China Shenzhen Institute for Advanced Study University of Electronic Science and Technology of ChinaShenzhen 518110China

设计廉价和高效的双功能催化剂应用于CO_(2)还原和O_(2)还原反应(CO_(2)RR和ORR)是实现碳中和的理想选择.因此,本文研制出铌原子分散固定在氮掺杂有序介孔碳(Nb-N-C)上的双功能CO_(2)RR和ORR催化剂用于锌-空气电池(ZAB)自驱动CO_(2)RR.... 详细信息

设计廉价和高效的双功能催化剂应用于CO_(2)还原和O_(2)还原反应(CO_(2)RR和ORR)是实现碳中和的理想选择.因此,本文研制出铌原子分散固定在氮掺杂有序介孔碳(Nb-N-C)上的双功能CO_(2)RR和ORR催化剂用于锌-空气电池(ZAB)自驱动CO_(2)RR.得益于高铌原子利用率和有序介孔结构,Nb-N-C催化剂展现出高达90%的CO法拉第效率,ORR的半波电位活性为0.84 V,ZAB的峰值功率活性为115.6 mW cm-2.此外,采用两个串联的ZABs单元作为自供能CO_(2)RR系统的电源,能够连续将C O_(2)转化为C O.该自供能系统前10小时的C O平均产率为3.75μmol h-1mg-1cat.理论计算表明,铌原子分散固定在氮掺杂的碳上形成Nb–N配位键,从而有效地降低CO_(2)RR的决速中间体*COOH和ORR的决速中间体*O的生成能垒.

关键词：有序介孔碳配位键还原反应双功能催化剂半波电位原子利用率氮掺杂能垒

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Formation of active oxygen species on single-atom Pt catalyst and promoted catalytic oxidation of toluene

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Nano Research 2020年第6期13卷 1544-1551页

作者： Shunzheng Zhao Yanfeng Wen Xijun Liu Xianyun Pen Fang Lü Fengyu Gao Xizhou Xie Chengcheng Du Honghong Yi Dongjuan Kang Xiaolong Tang Department of Environmental Engineering University of Science and Technology BeijingBeijing100083China Beijing Key Laboratory of Resource-oriented Treatment of Industrial Pollutants Beijing100083China Center for Electron Microscopy and Tianjin Key Lab of Advanced Functional Porous Materials Institute for New Energy Materials&Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin300384China

Catalytic oxidation of toluene over noble metal catalysts is a representative reaction for elimination of volatile organic compounds(VOCs).However,to fully understand the activation of molecular oxygen and the role of active oxygen species generated in this reaction is still a challenging ***,MgO nanosheets and single-atom Pt loaded MgO(Pt SA/MgO)nanosheets were synthesized and used as catalysts in toluene *** activation process of molecular oxygen and oxidation performance on the two catalysts were contrastively *** Pt SA/MgO exhibited significantly enhanced catalytic activity compared to *** oxygen vacancies can be easily generated on the Pt SA/MgO surface,which facilitate the activation of molecular oxygen and the formation of active oxygen *** on the experimental data and theoretical calculations,an active oxygen species promoted oxidation mechanism for toluene was *** the presence of H2O,the molecular oxygen is more favorable to be dissociated to generate•OH on the oxygen vacancies of the Pt SA/MgO surface,which is the dominant active oxygen *** anticipate that this work may shed light on further investigation of t10.1007/s12274-020-2765-1he oxidation mechanism of toluene and other VOCs over noble metal catalysts.

关键词： single-atom Pt activation of molecular oxygen oxygen vacancies active oxygen species oxidation of toluene

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富氧空位的非晶氧化铜高选择性电催化还原CO2制乙烯（英文）

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物理化学学报 2023年第2期39卷 106-114页

作者：韦天然张书胜刘倩邱园罗俊刘熙俊广西大学有色金属及材料加工新技术教育部重点实验室广西有色金属及特色材料加工重点实验室资源环境与材料学院郑州大学化学学院成都大学高等研究院电子科技大学深圳高等研究院天津理工大学新能源材料与低碳技术研究院材料科学与工程学院

过量化石能源的消耗导致大气中的二氧化碳含量不断上升,由此引发包括温室效应在内的环境问题。对此,常温常压下的电催化二氧化碳还原手段为制备高附加值的化工原料和实现碳循环提供了一种很有前景的技术储备。在众多的二氧化碳还原产物... 详细信息

过量化石能源的消耗导致大气中的二氧化碳含量不断上升,由此引发包括温室效应在内的环境问题。对此,常温常压下的电催化二氧化碳还原手段为制备高附加值的化工原料和实现碳循环提供了一种很有前景的技术储备。在众多的二氧化碳还原产物中,碳氢化合物尤其是乙烯,它作为塑料和其他化工产品的重要原料受到广泛的关注。电催化二氧化碳还原制乙烯工艺不仅可适配于现有的生产设备也可作为取代目前工业化的裂解方法。近年来,研究者们为了开发高效的电催化二氧化碳还原制乙烯催化剂开展了大量的研究。不过值得注意的是,大部分研究集中于铜基材料。尽管目前研究者取得了很多成果,但仍缺少可高选择性产乙烯的二氧化碳还原催化剂。如何设计出可活化二氧化碳分子,同时对*CO和*COH中间物有强吸附能力的催化剂是研究难点。针对此问题,本文中通过真空蒸镀的方法制备出一种富氧空位的非晶氧化铜纳米薄膜催化剂。受益于纳米薄膜的构建和氧空位的引入,该催化剂可快速进行电荷和物质的交换,并利于二氧化碳分子的吸附及优化还原中间产物的亲和力,进而表现出优异的电催化二氧化碳制乙烯的性能。结果表明,在加有0.1 mol·L-1碳酸氢钾溶液的H型电解池中测试中,该催化剂在相对于可逆氢电极电势为-1.3 V的产乙烯法拉第效率可达85%±3%。此外,该催化剂在长达48 h的电催化还原过程中仍可保持高的乙烯选择性。这些指标与已报道的最好的铜基催化剂的性能相当。另外,结构和化学手段表明该催化剂在电解反应中可保持良好的稳定性。进一步,我们测试了该催化剂在膜电极体系的性能,结果表明该催化剂的最大乙烯局部电流密度可达115.4 mA·cm-2(操作电压为-1.95 V),最高法拉第效率可达78%±2%(操作电压为-1.75 V)。理论和实验结果证明该催化剂的高乙烯选择性源于引入的氧空位不仅有利于二氧化碳分子的吸附,而且可增强对*CO和*COH的亲和力。本论文的研究不仅可激发学术界对高乙烯选择性的非晶铜基材料开发,同时在一定程度上提供有关电催化二氧化碳制乙烯的反应机制认识。

关键词：二氧化碳固定二碳产物电催化非晶催化剂铜氧化物

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Two-in-one solution using insect wings to produce graphene-graphite films for efficient electrocatalysis

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Nano Research 2019年第1期12卷 33-39页

作者： Huaiyu Li Lihan Zhang Long Li Chaowen Wu Yajiao Huo Ying Chen Xijun Liu Xiaoxing Ke Jun Luo Gustaaf Van Tendeloo Center for Electron Microscopy TUT-FEI Joint LabTianjin Key Lab of Advanced Functional Porous MaterialsInstitute for New Energy Materials&Low-Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China Institute of Microstructure and Property of Advanced Materials Beijing University of TechnologyBeijing 100124China EMAT Electron Microscopy for Materials ScienceUniversity of AntwerpGroenenborgerlaan 171B-2020 AntwerpBelgium Nanostructure Research Centre Wuhan University of TechnologyWuhan 430070China

Natural organisms contain rich elements and naturally optimized smart structures,both of which have inspired various innovative concepts and desig ns in human *** particular,several natural organisms have been used as element sources to synthesize low-cost and environmentally friendly electrocatalysts for the oxygen reduction reaction(ORR)in fuel cells and metal-air batteries,which are clean energy ***,to date,no naturally optimized smart structures have been employed in the synthesis of ORR catalysts,including graphene-based ***,we demonstrate a novel strategy to synthesize graphene-graphite films(GGFs)by heating butterfly wings coated with FeCI3 in N2,in which the full power of natural organisms is *** wings work not only as an element source for GGF generation but also as a porous supporting structure for effective nitrogen doping,two-dimensional spreading,and double-face exposure of the *** GGFs exhibit a half-wave potential of 0.942 V and a H2O2 yield of<0.07%for ORR electrocatalysis;these values are comparable to those for the best commercial Pt/C and all previously reported ORR catalysts in alkaline *** two-in-one strategy is also successful with cicada and dragonfly wings,indicating that it is a universal,green,and cost-effective method for developing high-performance graphene-based materials.

关键词： insect wings graphene graphite oxygen reduction reaction electrocatalysts

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高熵合金在水电解中的研究进展、基础与挑战

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Science China Materials 2023年第5期66卷 1681-1701页

作者：张泉廉康齐高璨张书胜刘倩罗扬罗俊刘熙俊 Institute for New Energy Materials&Low-Carbon Technologies School of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China MOE Key Laboratory of New Processing Technology for Non-Ferrous Metals and Materials and Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured MaterialsSchool of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China School of Materials Science and Engineering Tianjin University of TechnologyTianjin 300384China College of Chemistry Zhengzhou UniversityZhengzhou 450000China Institute for Advanced Study Chengdu UniversityChengdu 610106China Department of Materials ETH ZürichZürich 8093Switzerland Department of Physics City University of Hong KongHong Kong SAR 999077China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

氢能作为一种清洁能源,已成为全球能源战略的重要组成部分,也是实现全球“碳中和”的必要途径之一.在可再生电力的驱动下,水电解法有望成为实现“零碳”排放的一种理想的长期制氢方法.与传统合金相比,高熵合金由于其独特的结构特征,包... 详细信息

氢能作为一种清洁能源,已成为全球能源战略的重要组成部分,也是实现全球“碳中和”的必要途径之一.在可再生电力的驱动下,水电解法有望成为实现“零碳”排放的一种理想的长期制氢方法.与传统合金相比,高熵合金由于其独特的结构特征,包括占位无序和晶格有序,可提供更多的催化活性位点.它们在水解催化剂领域具有广泛的应用前景.本文综述了电解水的机理、水解过程中高熵合金的催化原理,以及高熵合金作为电解水催化剂的最新研究进展.总结了新型高熵合金设计方面存在的难点及其应用潜力,重点讨论了高熵合金在水解催化过程中表面形态和催化活性之间的联系.最后归纳了高熵合金的组成调控及其在水电解等新兴领域的可能应用前景.

关键词： high-entropy alloys electrolytic water splitting catalysts design hydrogen evolution reaction oxygen evolution reaction

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Engineering active sites of cathodic materials for high-performance Zn-nitrogen batteries

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Nano Research 2023年第7期16卷 9214-9230页

作者： Shanshan Chen Kang Lian Wenxian Liu Qian Liu Gaocan Qi Jun Luo Xijun Liu Institute for New Energy Materials and Low-Carbon Technologies Tianjin Key Lab for Photoelectric Materials&DevicesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China State Key Laboratory of Featured Metal Materials and Life-cycle Safety for Composite Structures School of ResourceEnvironments and MaterialsGuangxi UniversityNanning 530004China College of Materials Science and Engineering Zhejiang University of TechnologyHangzhou 310014China Institute for Advanced Study Chengdu UniversityChengdu 610106China ShenSi Lab Shenzhen Institute for Advanced StudyUniversity of Electronic Science and Technology of ChinaShenzhen 518110China

As an ideal carbon-free energy carrier,ammonia plays an indispensable role in modern *** conventional industrial synthesis of NH3 by the Haber-Bosch technique under harsh reaction conditions results in serious energy consumption and environmental ***,it is essential to develop NH3 synthesis tactics under benign *** synthesis of NH_(3) has the advantages of mild reaction conditions and environmental friendliness,and has become a hotspot for research in recent *** has been reported that zinc-nitrogen batteries(ZNBs),such as Zn-N_(2),Zn-NO,Zn-NO_(3)^(-),and Zn-NO_(2)^(-)batteries,can not only reduce nitrogenous species to ammonia but also have concomitant power ***,the common drawbacks of these battery systems are unsatisfactory power density and ammonia *** this review,the latest progress of ZNBs including the reaction mechanism of the battery and reactor design principles is systematically ***,active site engineering of cathode catalysts is discussed,including vacancy defects,chemical doping,and heterostructure ***,some insights are provided to improve the performance of ZNBs from a practical perspective of view.

关键词： Zn-nitrogen batteries nitrogen reduction electrocatalysis ammonia synthesis aqueous battery

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