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Rational design strategies of Cu-based electrocatalysts for CO_(2) electroreduction to C_(2) products

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Journal of Energy Chemistry 2022年第8期31卷 63-82,I0003页

作者： Shuo Liu Baoshan Zhang Lihong Zhang Jie Sun Key Laboratory for Green Chemical Technology of Ministry of Education School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China

Electrochemical reduction of CO_(2)(CO_(2)RR)to high value-added chemicals is an effective way to remove excess CO_(2) from the *** to the unique propensity of Cu for valuable hydrocarbons,Cu-based electrocatalysts are the most potential catalysts that allow the conversion of CO_(2) into a variety of C_(2) products such as ethylene and *** design of Cu-based catalysts can improve their directional selectivity to C_(2) ***,in this review,we summarize the recent progress in the mechanistic studies of Cu-based catalysts on reducing CO_(2) to C_(2) *** focus on three key strategies for efficiently enhancing electrocatalytic performance of Cu-based catalysts,including tuning electronic structure,surface structure,and coordination *** correlation between the structural characteristics of Cu-based catalysts and their activity and selectivity to C_(2) products is ***,we discuss the challenges in the field of CO_(2) electroreduction to C_(2) products and provide the perspectives to design efficient Cu-based catalysts in the future.

关键词： Carbon dioxide Cu-based catalysts Mechanisms Active site regulation

Integrated electrocatalysts derived from metal organic frameworks for gas-involved reactions

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Nano Materials Science 2023年第2期5卷 161-176页

作者： Yuke Song Wenfu Xie Mingfei Shao Xue Duan State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China

Integrated electrocatalysts(IECs)containing well-defined functional materials directly grown on the current collector have sparked increasing interest in the fields of electrocatalysis owing to efficient activity,high stability and the fact that they are easily assembled into ***,metal organic frameworks(MOFs)provide a promising platform for constructing advanced IECs because of their properties of low cost,large surface area and efficient structural *** this review,the design principles of state-of-the-art IECs based on MOFs are presented,including by hydrothermal/solvothermal,template-directed,electrospinning,electrodeposition and other *** high performance of MOF-derived IECs has also been demonstrated in electrocatalytic gasinvolved *** is promising for green energy storage and *** structure-activity relationship and performance improvement mechanism of IECs are uncovered by discussing some in situ technologies for ***,we provide an outlook on the challenges and prospects in this booming field.

关键词： Integrated electrocatalyst Metal organic framework Structure-activity relationship Gas-involved reaction

Layered Double Hydroxides for Oxygen Evolution Reaction towards Efficient Hydrogen Generation

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Energy Material Advances 2022年第1期2022卷 101-117页

作者： Xin Wan Yingjie Song Hua Zhou Mingfei Shao State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Electrochemical water splitting is one of the effective ways to obtain highly pure ***,as one of the two half reactions,oxygen evolution reaction(OER)has a high overpotential,resulting in the low-energy utilization ***,numerous electrocatalysts have been developed to reduce the energy barrier of *** them,layered double hydroxides(LDHs)are excellent OER electrocatalysts with flexible composition and structure,which have been widely investigated in the past *** studies have been focusing on the identification of active sites for LDHs during OER process,trying to reveal clear reaction mechanism for designing more efficient LDHs ***,this review tries to discuss the advances in identifying active site of LDHs based OER electrocatalysts for efficient hydrogen *** first introduce the effect of structure,composition,and defects to the OER performance of ***,main attention is paid on the active sites and mechanisms during OER,especially the coordination structures and catalytic mechanisms of active *** the end of this review,we put forward the existing problems and shortcomings in this fields,and propose the corresponding solutions,aiming to further promote the development of outstanding OER electrocatalysts towards efficient hydrogen production.

关键词： Oxygen hydroxide shortcomings

Layered double hydroxides functionalization toward rechargeable batteries Author links open overlay panel

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Particuology 2024年第8期91卷 138-154页

作者： Jianxiong Gao Bowen Jin Mingfei Shao State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Renewable Energy Research Institute Quzhou Institute for Innovation in Resource Chemical EngineeringQuzhou324000China

Layered double hydroxides(LDHs),known as typical two-dimensional materials with unique physicochemical properties,are regarded as promising candidates in energy storage ***,some inherent defects,such as poor conductivity and limited active sites,hinder the further development of ***,various functionalization strategies(e.g.,intercalation of guest molecules;metal ions doping and defect introduction of host layer;exfoliation to monolayer;hybridization with functional materials;construction of hierarchical structure;interface engineering and phase transformation)have been used to modify the characteristics of LDHs,which provides guidance for designing novel *** this review,we discuss how these strategies improve the properties of LDH-based materials,which are expected to possess high electronic and ionic conductivity,high specific surface area and high mechanical and chemical stability ***,the application of LDH-based materials in advanced energy conversion and storage techniques,including metal-ions batteries,lithium-sulfur batteries and metal-air batteries,have been comprehensively summarized.

关键词： Layered double hydroxide Functionalization strategy Rechargeable battery

Metal vacancy-enriched layered double hydroxide for biomass molecule electrooxidation coupled with hydrogen production

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Fundamental Research 2024年第1期4卷 69-76页

作者： Yingjie Song Shan Jiang Yeheng He Yu Wu Xin Wan Wenfu Xie Jingjing Wang Zhenhua Li Haohong Duan Mingfei Shao State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China PetroChina Petrochemical Research Institute China National Petroleum CorporationBeijing 100195China Department of Chemistry Tsinghua UniversityBeijing 100084China

The electrochemical oxidation of biomass molecules coupling with hydrogen production is a promising strategy to obtain both green energy and value-added chemicals;however,this strategy is limited by the competing oxygen evolution reactions and high energy ***,we report a hierarchical CoNi layered double hydroxides(LDHs)electrocatalyst with abundant Ni vacancies for the efficient anodic oxidation of 5-hydroxymethylfurfural(HMF)and cathodic hydrogen *** unique hierarchical nanosheet structure and Ni vacancies provide outstanding activity and selectivity toward several biomass molecules because of the finely regulated electronic structure and highly-exposed active *** particular,a high faradaic efficiency(FE)at a high current density(99%at 100 mA cm^(-2))is achieved for HMF oxidation,and a two-electrode electrolyzer is assembled based on the Ni vacancies-enriched LDH,which realized a continuous synthesis of highly-pure 2,5-furandicarboxylic acid products with high yields(95%)and FE(90%).

关键词： Layered double hydroxides Biomass upgrading 5-hydroxymethylfurfural Hydrogen production Coupled oxidation

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水泥生料共热耦合原位加氢制合成气

洁净煤技术 2024年第4期30卷 90-101页

作者：张卫涛于少康徐明董猛郭大冰杨宇森邵明飞段雪北京化工大学化工资源有效利用国家重点实验室北京100029 衢州资源化工创新研究院浙江衢州324003 东北林业大学化学化工与资源利用学院黑龙江哈尔滨150006

水泥工业是世界第三大能源消耗行业和第二大CO_(2)排放行业,占全球CO_(2)排放的7%。水泥生料(CaCO_(3)、Fe_(2)O_(3)、Al_(2)O_(3)和SiO_(2)的混合物)通过高温(>900℃)煅烧得到水泥熟料,此过程能耗高且释放大量CO_(2)。基于双碳背景,通... 详细信息

水泥工业是世界第三大能源消耗行业和第二大CO_(2)排放行业,占全球CO_(2)排放的7%。水泥生料(CaCO_(3)、Fe_(2)O_(3)、Al_(2)O_(3)和SiO_(2)的混合物)通过高温(>900℃)煅烧得到水泥熟料,此过程能耗高且释放大量CO_(2)。基于双碳背景,通过球磨法制备水泥生料,采用碳酸盐共热耦合原位加氢还原的创新策略,实现在700℃下水泥生料原位加氢生成CO,其选择性可达94.8%,CO生成速率达0.76 mmol/min,显著降低了碳酸盐的热解温度并抑制了CO_(2)排放,同时获得了均匀多孔的CaO颗粒。采用X射线粉末衍射(XRD)、比表面及孔径分析(BET)、扫描电子显微镜(SEM)、拉曼光谱(Raman)及原位漫反射傅里叶变换红外光谱(In situ DRIFTS)等表征手段,重点探究了反应温度和水泥不同组分(Fe、Si和Al)等因素对碳酸盐加氢性能的影响。结果表明,Fe元素有助于提升CO产物选择性且生成少量甲烷,Si和Al元素的加入降低了碳酸盐加氢反应速率。In situ DRIFTS表明水泥生料加氢生成CO可能遵循甲酸盐中间物种机制。本研究通过水泥生料共热耦合原位加氢制备合成气,实现水泥工业源头降耗与减排增效,为低碳水泥熟料的制备技术提供了新策略与理论依据。

关键词：水泥生料碳酸盐共热耦合碳减排合成气

光电解水制氢耦合生物质醇/醛氧化的研究进展

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高等学校化学学报 2022年第2期43卷 172-181页

作者：陈望松罗兰刘玉广周华孔祥贵栗振华段昊泓北京化工大学化学学院化工资源有效利用国家重点实验室北京100029 清华大学化学系北京100084

生物质醇/醛是一类重要的生物基平台化合物,通过催化氧化重整可将其进一步转化为高值含氧化学品或燃料.太阳能驱动的光电催化技术是实现生物质醇/醛氧化最为绿色高效的途径之一.与传统光电解水制氢相比,利用生物质醇/醛氧化来替代阳极... 详细信息

生物质醇/醛是一类重要的生物基平台化合物,通过催化氧化重整可将其进一步转化为高值含氧化学品或燃料.太阳能驱动的光电催化技术是实现生物质醇/醛氧化最为绿色高效的途径之一.与传统光电解水制氢相比,利用生物质醇/醛氧化来替代阳极析氧过程不仅可以提高阳极产物的附加值,同时可以提升太阳能到氢能的转化效率.因此,光电解水制氢耦合生物质醇/醛氧化对绿氢提效降本和高值化学品合成具有重要意义.本文综合评述了光电解水制氢耦合生物质醇/醛的氧化反应机理,总结了目前光电催化技术在生物质醇/醛氧化方面的研究进展,最后对该领域所面临的机遇和挑战进行了展望.

关键词：光电解水生物质催化氧化制氢耦合反应

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镍钒水滑石电极用于可放大电催化5-羟甲基糠醛氧化耦合产氢

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物理化学学报 2024年第9期40卷 56-58页

作者：李美然宋英杰万鑫李洋罗毅奇贺业亨夏博文周华邵明飞北京化工大学化学学院化工资源有效利用国家重点实验室北京100029 中国石油石油化工研究院北京100195 衢州资源化工创新研究院浙江衢州324000

可再生能源驱动的电催化水裂解是获取绿氢的重要途径,但受到缓慢的阳极析氧反应(OER)限制。使用热力学有利的5-羟甲基糠醛氧化反应(HMFOR)代替OER的电解水制氢耦合氧化策略提供了一种降低能耗的有效策略,同时可以生产高附加值的有机含... 详细信息

可再生能源驱动的电催化水裂解是获取绿氢的重要途径,但受到缓慢的阳极析氧反应(OER)限制。使用热力学有利的5-羟甲基糠醛氧化反应(HMFOR)代替OER的电解水制氢耦合氧化策略提供了一种降低能耗的有效策略,同时可以生产高附加值的有机含氧化合物,如2,5-呋喃二甲酸(FDCA)。在该领域,大量工作集中于催化剂工程以获得更好的催化活性和产物选择性。然而,很少有研究关注到5-羟甲基糠醛(HMF)的规模化氧化制备FDCA。为此,我们合成了一种镍钒水滑石(NiV-LDH)催化剂用于高效HMFOR,在1.52 V ***(可逆氢电极)下,电流密度达到100 mA·cm^(-2) FDCA的法拉第效率高达94.6%。与OER相比,HMFOR将对应的氢气生产率提高了两倍。作为概念验证,我们使用流动反应器展示了连续且可规模化的HMFOR,在10 A条件下,实现了94.8%的高HMF单程转化率和98.5%的高FDCA选择性。

关键词：电催化水分解耦合制氢层状双金属氢氧化物 5-羟甲基糠醛 2,5-呋喃二甲酸

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碱性电解水高效制氢

电化学 2022年第10期28卷 51-68页

作者：谢文富邵明飞北京化工大学化学学院化工资源有效利用国家重点实验室北京100029

与传统化石能源制氢技术相比,利用可再生能源驱动电解水制氢技术具有绿色可持续和制氢效率高等优势,被认为是目前最具前景的制氢方式。然而,由于电解水两极反应动力学缓慢、催化剂稳定性较差,限制了其大规模发展。此外,阳极析氧反应存... 详细信息

与传统化石能源制氢技术相比,利用可再生能源驱动电解水制氢技术具有绿色可持续和制氢效率高等优势,被认为是目前最具前景的制氢方式。然而,由于电解水两极反应动力学缓慢、催化剂稳定性较差,限制了其大规模发展。此外,阳极析氧反应存在较高的过电势,从而导致当前制氢能耗与成本较高,严重制约了其商业化应用。为了解决上述问题与挑战,本文对当前发展较为成熟的碱性电解水技术进行了综合讨论与分析。首先,对电解水发展历程中的重要节点进行了总结,便于读者了解该领域。进一步,从电催化剂、电极、反应和系统的角度深入总结了提升电解水制氢性能的有效策略。作者分别介绍了近年来层状双金属氢氧化物基电解水催化剂、电解水制氢耦合氧化反应以及可再生能源驱动的电解水系统的重要研究进展;同时对结构化催化剂在电解水应用中的构效关系进行了深入分析。最后,对该领域存在的挑战和未来发展方向进行了展望,希望能为氢能的发展和推广提供一定的思路。

关键词：电解水制氢结构化电极耦合反应