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类金属WO_(2)/g-C_(3)N_(4)复合光催化剂的构造及其优异的光催化性能

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Chinese Journal of Catalysis 2023年第4期47卷 161-170页

作者：李宁高雪云苏俊珲高旸钦戈磊中国石油大学(北京)重质油加工国家重点实验室北京102249 中国石油大学(北京)新能源与材料学院材料科学与工程系北京102249

随着化石燃料快速消耗和环境污染日益严峻,高效光催化产氢技术作为最有前景的绿色能源技术之一而备受关注.作为典型的2D纳米片,g-C_(3)N_(4)具有很多适合应用在光催化领域的特性,如可见光效应、大比表面积和环境友好等,但单一g-C_(3)N_... 详细信息

随着化石燃料快速消耗和环境污染日益严峻,高效光催化产氢技术作为最有前景的绿色能源技术之一而备受关注.作为典型的2D纳米片,g-C_(3)N_(4)具有很多适合应用在光催化领域的特性,如可见光效应、大比表面积和环境友好等,但单一g-C_(3)N_(4)的载流子复合率高,光催化性能不佳.研究者尝试负载贵金属(如Pt,Ag,Au等),利用贵金属功函数较高,可以快速捕获g-C_(3)N_(4)表面的光生电子,从而有效抑制光生载流子的复合;但其成本较高,限制了该技术的产业化.目前类金属材料(MoO_(2),NbO_(2),WO_(2)等)不仅表现出类似贵金属的特性,且价格低廉,有望替代贵金属.因此,引入类金属助催化剂是实现高载流子浓度和宽光谱照射下强光子吸收的好方法.本文设计并制备了类金属WO_(2)/g-C_(3)N_(4)纳米复合物,其表现出了较好的光催化性能:在可见光照射2h,4 wt%WO_(2)/g-C_(3)N_(4)的光催化降解效率高达96%;同时,4 wt%WO_(2)/g-C_(3)N_(4)/Pt产氢效率高达2436.9μmolg^(-1)h^(-1),是未改性样品3 wt%Pt/g-C_(3)N_(4)的2.55倍和非贵金属样品WO_(2)/g-C_(3)N_(4)的6.18倍,且表现出很好的循环稳定性.紫外可见漫反射光谱和态密度计算结果表明,WO_(2)具有非常窄的带隙,可吸收200-800 nm的宽范围可见光.实验测试和理论计算结果表明,WO_(2)因带隙较窄而表现出类金属特性,即在WO_(2)/g-C_(3)N_(4)界面,WO_(2)快速捕获电子,从而抑制光生载流子的复合.类金属WO_(2)因具有较低的功函数而表现出比贵金属Pt低的捕获光生电子活性.综上,本文为合理设计助催化剂/半导体,实现高效的光催化性能提供了新视角.

关键词： g-C_(3)N_(4) 类金属WO_(2) 光催化产氢性能光催化降解非贵金属光催化剂

过渡金属硫化物相关电催化剂的设计与应用研究

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Chinese Journal of Catalysis 2023年第1期44卷 7-49页

作者：苏慧姜静宋少佳安博涵李宁高旸钦戈磊中国石油大学(北京)新能源与材料学院重质油国家重点实验室北京102249 中国石油大学(北京)新能源与材料学院材料科学与工程系北京102249 中国石油大学(北京)理学院应用化学系北京102249

自从国际社会提出“碳达峰、碳中和”目标以来,人们越来越意识到节约资源、保护环境、开发新能源的必要性.氢能(H_(2))作为最具竞争力的清洁能源之一,引起了研究人员的广泛关注.电化学全解水被认为是一种利用风能和太阳能产生氢气的有... 详细信息

自从国际社会提出“碳达峰、碳中和”目标以来,人们越来越意识到节约资源、保护环境、开发新能源的必要性.氢能(H_(2))作为最具竞争力的清洁能源之一,引起了研究人员的广泛关注.电化学全解水被认为是一种利用风能和太阳能产生氢气的有效技术,其主要由两个半反应组成:析氧反应(OER)和析氢反应(HER).然而,在实际工业化生产过程中阳极反应动力学OER慢,能量转换效率低,阴极反应稳定性差,导致经济效益不理想,因此,急需开发和探索耐久高效的电催化剂.过渡金属硫化物因具有独特的结构特征、丰富的活性位点和可调控的电子性质和组成,而被广泛用于电化学全解水制氢.本文综述了过渡金属硫化物的合成方法,一般包括:水热(溶剂热)法、电化学沉积法、液相剥离法、化学气相沉积法和球磨法,并概述了不同方法的基本概念、合成步骤以及优缺点.总结了近年用于电催化领域中典型单一硫化物(包括MoS_(2),WS_(2),Co3S_(4),Ni_(3)S_(2)等)材料的合成方法和机理,明确了S元素在整个电催化过程中的重要作用.针对单一硫化物稳定性差、活性位点少、电化学活性不高的缺点,详细总结了双金属、多金属以及单原子、双原子硫化物的催化机理和催化性能.当采用复合、引入缺陷、空缺和形态调节等手段修饰时,能够有效调控金属硫化物的电子结构,增加活性位点数量,优化反应中间体的吸附能,降低OER过程的能垒,从而使多金属硫化物具有优异的电化学性能.最后,通过一些典型的研究结果揭示了过渡金属硫化物在水分子分裂过程中的结构特性变化原理,特别是对于多金属硫化物,活性位点可以是金属阳离子,而其他金属的引入将在一定程度上改变活性中心附近的电子结构和配位环境,进而改善材料的催化性能.尽管过渡金属硫化物在电催化领域的应用研究取得了一系列进展,但仍存在诸多挑战,距实际应用仍有较大差距.需要综合考虑经济、高性能、稳定性和环境友好等因素进行过渡金属硫化物催化材料的设计、制备和性能调控,并为大规模应用提供基础.同时,深入探索电催化机理有利于设计高效电催化剂和推动电催化领域的持续发展.综上,本文为新型电催化材料的制备和电催化全解水机理的深入研究提供一定的参考.

关键词：过渡金属硫化物析氢反应析氧反应全解水电催化

Design and applications of hollow‐structured nanomaterials for photocatalytic H2 evolution and CO2 reduction

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Chinese Journal of Catalysis 2022年第3期43卷 679-707页

作者： Xuli Li Ning Li Yangqin Gao Lei Ge State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China Department of Materials Science and Engineering College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China

Photocatalysis is considered a prospective way to alleviate the energy crisis and environmental *** is therefore extremely important to design highly efficient photocatalysts for catalytic *** recent years,hollow‐structured materials have attracted considerable interest for application in energy conversion fields owing to their large specific surface areas,improved light absorption,and shortened charge carrier transfer *** they contain inner and outer surfaces,hollow‐structured materials can provide a superior platform for the deposition of other components.A number of hollow‐structured hierarchical systems have been designed and fabricated in recent *** is important to rationally design and construct complex hierarchical *** this review,general preparation approaches for hollow‐structured materials are presented,followed by a summary of the recent synthesis methods and mechanisms of typical hollow‐structured materials for applications in the photocatalytic *** hollow‐structured hierarchical photocatalysts are classified into two types,hollow cocatalyst‐based and hollow host photocatalyst‐based,and the design principle and analysis of the photocatalytic reaction mechanism for photocatalytic H2 evolution and CO_(2) reduction are also *** effects of hollow‐structured materials have also been *** review provides a reference for the rational construction of advanced,highly efficient photocatalytic materials.

关键词： Hollow structure Photocatalysis H_(2)evolution CO_(2)reduction Design principle

The roles and mechanism of cocatalysts in photocatalytic water splitting to produce hydrogen

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Chinese Journal of Catalysis 2020年第4期41卷 642-671页

作者： Nan Xiao Songsong Li Xuli Li Lei Ge Yangqin Gao Ning Li State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China Department of Materials Science and Engineering College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China

Photocatalytic hydrogen(H2)evolution via water spilling over semiconductors has been considered to be one of the most promising strategies for sustainable energy supply in the future to provide non-pollution and renewable *** key to efficient conversion of solar-chemical energy is the design of an efficient structure for high charge separation and ***,cocatalysts are necessary in boosting photocatalytic H2 *** date,semiconductor photocatalysts have been modified by various cocatalysts due to the extended light harvest,enhanced charge carrier separation efficiency and improved *** review focuses on recent developments of cocatalysts in photocatalytic H2 evolution,the roles and mechanism of the cocatalysts are discussed in *** cocatalysts can be divided into the following categories:metal/alloy cocatalysts,metal phosphides cocatalysts,metal oxide/hydroxide cocatalysts,carbon-based cocatalysts,dual cocatalysts,Z-scheme cocatalysts and MOFs *** future research and forecast for photocatalytic hydrogen generation are also suggested.

关键词： Cocatalysts Photocatalytsts Hydrogen evolution Charge separation Water splitting

产学合作模式在材料专业人才培养机制中的探索

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科教导刊 2020年第19期 58-59页

作者：戈磊李宁高旸钦邱萍中国石油大学(北京)新能源与材料学院北京102249

本文针对目前工科专业人才培养与社会需求脱节问题,在材料科学与工程专业人才培养过程中,探索了一系列的产学合作的改革。以培养创新型和应用型人才为核心,加深校企协同合作,共建专业课程,全方位深入教学全过程,提升教师工程素养,优化... 详细信息

本文针对目前工科专业人才培养与社会需求脱节问题,在材料科学与工程专业人才培养过程中,探索了一系列的产学合作的改革。以培养创新型和应用型人才为核心,加深校企协同合作,共建专业课程,全方位深入教学全过程,提升教师工程素养,优化毕业生质量评估体系,有效促进学校、学生、企业等多方共赢。

关键词：材料科学与工程专业产学合作人才培养

高效非贵金属助催化剂的设计及光催化产氢性能研究

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高效非贵金属助催化剂的设计及光催化产氢性能研究

Pt/Bi_(24)O_(31)Cl_(10) composite nanosheets with significantly enhanced photocatalytic activity under visible light irradiation

2018第二届全国光催化材料创新与应用学术研讨会

作者：戈磊李松松许浩代东升高旸钦李宁中国石油大学(北京)理学院材料科学与工程系

光催化材料可利用清洁的太阳能光解水制氢和降解环境污染物等,设计与合成新型高效的光催化材料是目前光催化领域迫切而具有挑战性的重要课题。本文通过深入研究复合光催化剂的可控合成,探讨了助催化剂结构和光催化活性之间的关系,有效...

光催化材料可利用清洁的太阳能光解水制氢和降解环境污染物等,设计与合成新型高效的光催化材料是目前光催化领域迫切而具有挑战性的重要课题。本文通过深入研究复合光催化剂的可控合成,探讨了助催化剂结构和光催化活性之间的关系,有效提升了半导体光催化材料的性能和光量子效率,并拓宽了光催化剂在能源危机缓解和环境污染控制领域内的应用:

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来源： cnki会议评论

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Chinese Journal of Catalysis 2019年第5期40卷 713-721页

作者： Boran Xu Juan Li Lu Liu Yandong Li Shaohui Guo Yangqin Gao Ning Li Lei Ge State Key Laboratory of Heavy Oil Processing College of Science China University of Petroleum Beijing Beijing 102249 Department of Materials Science and Engineering College of Science China University of Petroleum Beijing Beijing 102249

Efficient composite semiconductor photocatalysts are highly desirable for the visible-light-driven degradation of organic pollutants. In this study, Bi24O31Cl10 photocatalyst was prepared via a hydrothermal method and modified with Pt nanoparticles (NPs) through a facile deposition procedure. The composite photocatalyst was characterized by X-ray diffraction, transmission electronic microscopy, X-ray photoelectron spectroscopy, UV-vis diffusion reflectance spectroscopy, photoluminescence spectroscopy, and electron spin resonance. The 1.0 wt% Pt/Bi24O31Cl10 photocatalyst showed the highest activity for the degradation of methyl orange under visible light (source: 300 W Xe lamp coupled with a UV-cutoff filter), and the photocatalytic degradation efficiency improved about 2.2 times compared to that of pure Bi24O31Cl10. The composite photocatalyst could maintain most of its activity after four runs of the photocatalytic experimental cycle. This study could provide a novel insight for the modification of other desirable semiconductor materials to achieve high photocatalytic activities.

关键词： Bismuth-based oxyhalide Photocatalyst Bi24O31Cl10 Methyl orange degradation

Synthesis of ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite materials with significantly improved photocatalytic H_(2)production performance

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Chinese Journal of Catalysis 2022年第5期43卷 1295-1305页

作者： Aixia Wang Linhe Zhang Xuli Li Yangqin Gao Ning Li Guiwu Lu Lei Ge State Key Laboratory of Heavy Oil Processing College of New Energy and MaterialsChina University of Petroleum BeijingBeijing 102249China College of Science China University of Petroleum BeijingBeijing 102249China

The design and construction of low‐cost and high‐performance hybrid materials for the photocatalytic hydrogen production reaction(HER)are extremely important for the large‐scale application of hydrogen ***‐organic frameworks(MOFs)are considered to be potential photocatalytic ***,monodisperse,small size,non‐precious metal transition metal phosphide Ni2P is encapsulated into a typical MOF(UiO‐66‐NH2)as a hybrid core‐shell cocatalyst to modify Zn_(0.5)Cd_(0.5)S for photocatalytic hydrogen ***2P is wrapped in UiO‐66‐NH_(2)via an in situ solvothermal method,and Zn_(0.5)Cd_(0.5)S sulfide is decorated with a core‐shell Ni_(2)P@UiO‐66‐NH_(2)cocatalyst to obtain ternary Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S composite *** and chemical characterization confirms that the ternary composites have good kinetic hydrogen production *** hydrogen production rate of 10%10 mg Ni_(2)P@UiO‐66‐NH_(2)/Zn_(0.5)Cd_(0.5)S reaches 40.91 mmol·g^(–1)·h^(–1)with an apparent quantum efficiency at 420 nm of 13.57%.The addition of 10 mg Ni_(2)P@UiO‐66‐NH_(2)increases the surface area of the ternary material,providing abundant reaction sites and forming an efficient charge transfer channel,which is conducive to efficient hydrogen production by the ternary *** is shown that the formation of a ternary composite system is beneficial to the occurrence of an efficient catalytic *** study provides a new perspective for the construction of high‐performance photocatalytic materials.

关键词： Ni2P UiO‐66‐NH2 Zn0.5Cd0.5S Hydrogen evolution Ternary photocatalyst

Novel PtPd alloy nanoparticle-decorated g-C_3N_4 nanosheets with enhanced photocatalytic activity for H_2 evolution under visible light irradiation

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Chinese Journal of Catalysis 2019年第3期40卷 352-361页

作者： Nan Xiao Songsong Li Shuang Liu Boran Xu Yandong Li Yangqin Gao Lei Ge Guiwu Lu State Key Laboratory of Heavy Oil Processing China University of Petroleum Beijing Beijing 102249 China College of New Energy and Materials China University of Petroleum Beijing Beijing 102249 China

PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C3N4) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H2 evolution of the g-C3N4 nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C3N4 composite photocatalyst gave a maximum H2 production rate of 1600.8 μmol g^–1 h^–1. Furthermore, when K2HPO4 was added to the reaction system, the H2 production rate increased to 2885.0 μmol g^–1 h^–1. The PtPd/g-C3N4 photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C3N4 helps to greatly improve the photocatalytic activity of the composite photocatalyst.

关键词： g-C3N4 nanosheets PtPd alloy nanoparticles H2 evolution Photocatalysis