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Flower-like NiCo_(2)S_(4)/NiFeP/NF composite material as an effective electrocatalyst with high overall water splitting performance

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Chinese Chemical Letters 2022年第9期33卷 4367-4374页

作者： Jing Jiang Fengyan Li Hui Su yangqin gao Ning Li 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

Rational design and building of high efficiency,secure and inexpensive electrocatalyst is a pressing demand and performance to promote sustainable improvement of hydrogen *** bifunctional electrocatalysts for oxygen evolution reaction(OER)and hydrogen evolution response(HER)with high catalytic performance and steadiness in the equal electrolyte are extra treasured and ***,a unique three-dimensional(3D)structure electrocatalyst for NiCo_(2)S_(4)growing on the flower-like NiFeP was designed and synthesized in this *** results show that the flower-like NiCo_(2)S_(4)/NiFeP/NF composite electrocatalyst has large specific surface area,appropriate electrical conductivity,and greater lively websites uncovered in the three-dimensional structure,and affords extraordinary electrocatalytic overall performance for the ordinary water *** alkaline solution,the OER and HER overpotentials of NiCo_(2)S_(4)/NiFeP/NF only need 293 mV and 205 mV overpotential to provide the current densities of 100 mA/cm^(2)and 50 mA/cm^(2),*** high electrocatalytic activity exceeds the catalytic activity of most nickel-iron based electrocatalysts for OER and HER ***,the optimized NiCo_(2)S_(4)/NiFeP/NF sample has higher stability(24 h)at 1.560 and 10 mA/cm^(2),which extensively speeds up the overall water splitting *** view of the above performance,this work offers a fine approach for the further improvement of low fee and excessive effectivity electrocatalyst.

关键词： NiCo_(2)S_(4) Electrocatalyst NiFeP Hydrogen evolution reaction Water splitting

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W-doped FeNi_(2)S_(4)/Ni_(3)S_(2)/NF with interfacial effect as efficient bifunctional electrocatalyst for overall water splitting

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Nano Research 2023年第10期16卷 12116-12125页

作者： Jing Jiang Hui Su Shaojia Song Weilong Liu 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

Given the current shortage of resources and environmental pollution,rationally designing and developing low-cost and highefficiency bifunctional electrocatalysts is an urgent and challenging *** is widely recognized that element doping can effectively improve the electrocatalytic activity by adjusting the microstructure,morphology,and electronic ***,this work rationally designs and prepares three-dimensional flower-like structured W-doped FeNi_(2)S_(4)/Ni_(3)S_(2)/NF heterojunctions as efficient bifunctional electrocatalysts for overall water *** 1 M KOH,the prepared W-FeNi_(2)S_(4)/Ni_(3)S_(2)/NF electrocatalyst can effectively drive both hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)processes,and only needs overpotentials of 93 and 210 mV to reach current densities of 10 and 50 mA·cm^(−2).In the double electrode cell composed by WFeNi_(2)S_(4)/Ni_(3)S_(2)/NF electrocatalyst,a low cell voltage of 1.52 V was required to reach a current density of 10 mA·cm^(−2),and 91.6%of this value was preserved after 24 h electrolysis *** performance of FeNi_(2)S_(4)/Ni_(3)S_(2)/NF electrocatalyst is superior to most of the current bifunctional electrocatalytic *** functional theory(DFT)theoretical calculations also revealed a more intense electron transfer process that can be facilitated by constructing FeNi_(2)S_(4)and Ni_(3)S_(2)/NF interface,which may be the main reason for the archived excellent electrochemical performance.

关键词： bifunctional electrocatalysts water splitting density functional theory(DFT)calculation oxygen evolution reaction(OER)

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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

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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

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Novel indirect Z-scheme g-C3N4/Bi2MoO6/Bi hollow microsphere heterojunctions with SPR-promoted visible absorption and highly enhanced photocatalytic performance

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Chinese Journal of Catalysis 2020年第3期41卷 426-434页

作者： Ning Li Hang gao Xin Wang Sujun Zhao Da Lv Guoqing Yang Xueyun gao Haikuan Fan yangqin gao Lei Ge State Key Laboratory of Heavy Oil Processing China University of Petroleum BeijingNo.18 Fuxue RDBeijing 102249China Department of Materials Science and Engineering College of New Energy and MaterialChina University of Petroleum BeijingNo.18 Fuxue RDBeijing 102249China Beijing Key Laboratory of Failure Corrosionand Protection of Oil/Gas FacilitiesCollege of New Energy and MaterialChina University of Petroleum BeijingBeijing 102249China

The surface plasmonic resonance(SPR)effect of Bi can effectively improve the light absorption abilities and photogenerated charge carrier separation *** this study,a novel ternary heterojunction of g-C3N4/Bi2MoO6/Bi(CN/BMO/Bi)hollow microsphere was successfully fabricated through solvothermal and in situ reduction *** results revealed that the optimal ternary 0.4 CN/BMO/9 Bi photocatalyst exhibited the highest photocatalytic efficiency toward rhodamine B(RhB)degradation with nine times that of pure *** DRS and valence band of the X-ray photoelectron spectroscopy spectrum demonstrate that the band structure of 0.4 CN/BMO/9 Bi is a z-scheme *** experiments also provided solid evidence that the·O^2-(at-0.33 eV)is the main species during dye degradation,and the conduction band of g-C3N4 is only the reaction site,demonstrating that the transfer of photogenerated charge carriers of g-C3N4/Bi2 MoO 6/Bi is through an indirect z-scheme ***,the enhanced photocatalytic performance was mainly ascribed to the synergetic effect of heterojunction structures between g-C3N4 and Bi2MoO6 and the SPR effect of Bi doping,resulting in better optical absorption ability and a lower combination rate of photogenerated charge *** findings in this work provide insight into the synergism of heterostructures and the SPR absorption ability in wastewater treatment.

关键词： g-C3N4/Bi2MoO6/Bi Z-scheme catalyst Surface plasmonic resonance effect Rhodamine B Visible light

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Atomic orbitals modulated dual functional bimetallic phosphides derived from MOF on MOF structure for boosting high efficient overall water splitting

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Chinese Journal of Catalysis 2024年第10期65卷 113-125页

作者： Bohan An Weilong Liu Jipeng Dong 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

The electronic modulation characteristics of efficient metal phosphide electrocatalysts can be utilized to tune the performance of oxygen evolution reaction(OER).However,improving the overall water splitting performance remains a challenging *** building metal organic framework(MOF)on MOF heterostructures,an efficient strategy for controlling the electrical structure of MOFs was presented in this ***-67 was in-situ synthesized on MIL-88(Fe)using a two-step self-assembly method,followed by low-temperature phosphorization to ultimately synthesize FeP-CoP_(3)bimetallic *** combining atomic orbital theory and theoretical calculations(density functional theory),the results reveal the successful modulation of electronic orbitals in FeP-CoP_(3)bimetallic phosphides,which are synthesized from MOF on MOF *** synergistic impact of the metal center Co species and the phase conjugation of both kinds of MOFs are responsible for this regulatory ***,the catalyst demonstrates excellent properties,demonstrating HER 81 mV(η10)in a 1.0 mol L^(−1)KOH solution and OER 239 mV(η50)low *** FeP-CoP_(3)linked dual electrode alkaline batteries,which are bifunctional electrocatalysts,have a good electrocatalytic ability and may last for 50 *** require just 1.49 V(η50)for total water *** this technique,the electrical structure of electrocatalysts may be altered to increase catalytic activity.

关键词： Transition metal phosphides MOF on MOF Atomic orbital theory Density functional theory calculation

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

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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

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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

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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

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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

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