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石墨炔在光催化中的应用

硅酸盐学报 2023年第1期51卷 106-116页

作者：靳治良北方民族大学化学与化学工程学院宁夏太阳能化学转化技术重点实验室国家民委化工技术基础重点实验室银川750021

石墨炔是一种新型碳的同素异形体,其独特的结构使得该物质具有理想的高强度、导电性、导热性、透光性和高载流子迁移率、热导率等。石墨炔具有天然的带隙,属于本征半导体,具有特别的电荷输运性能。石墨炔与无带隙的石墨烯相比,在0.45~1.... 详细信息

石墨炔是一种新型碳的同素异形体,其独特的结构使得该物质具有理想的高强度、导电性、导热性、透光性和高载流子迁移率、热导率等。石墨炔具有天然的带隙,属于本征半导体,具有特别的电荷输运性能。石墨炔与无带隙的石墨烯相比,在0.45~1.30 eV范围内显示出带隙,这使其在电子、催化、光学和机械方面具有强大的应用潜能,为碳材料的基础和应用研究提供新的空间、带来了新的内涵,引起了广泛的关注。此外,石墨炔在Fermi能级上下附近具有2个不同的Dirac锥,这表示石墨炔为自掺杂(self-doped)半导体,原本就具有电荷载流子,不需要像石墨烯一样要通过额外掺杂实现。石墨炔是十分契合的潜在的且卓越的光催化材料,理论上只需修饰构建活性位点即可高效光诱导反应。

关键词：石墨炔制备光催化产氢

Efficient photocatalytic hydrogen evolution over graphdiyne boosted with a cobalt sulfide formed S-scheme heterojunction

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Chinese Journal of Catalysis 2022年第2期43卷 303-315页

作者： zhiliang jin Hongying Li Junke Li School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021NingxiaChina

Graphdiyne(GDY,g-C_(n)H_(2n-2)),a novel two-dimensional carbon hybrid material,has attracted significant attention owing to its unique and excellent *** a new type of carbon material,GDY has a layered structure and can be used in the field of photocatalytic water ***,herein,new progress in the preparation of graphene using Cu I powder as a catalytic material and the combination of a facile hydrothermal method to prepare a new composite material,Co_(9)S_(8)-GDY-Cu I,is *** hydrogen production activity of Co9S8-GDY-Cu I in the sensitization system reached 1411.82μmol g^(-1) h^(-1),which is 10.29 times that of pure GDY.A series of characterization techniques were used to provide evidence for the successful preparation of the material and its superior photocatalytic *** spectroscopy showed that the material contains acetylenic bonds,and the X-ray photoelectron spectroscopy carbon fitting peaks indicated the presence of C-C(sp^(2))and C-C(sp),further demonstrating that GDY was successfully prepared.A possible reaction mechanism was proposed by making use of UV-visible diffuse reflectance and Mott-Schottky *** results showed that a double S-scheme heterojunction was constructed between the samples,which effectively accelerated the separation and transfer of *** addition,the introduction of Co9S8 nanoparticles greatly improved the visible light absorption capacity of Co_(9)S_(8)-GDY-Cu *** spectroscopy and related electrochemical characterization further proved that recombination of the electron-hole pairs in the composite material was effectively suppressed.

关键词： Graphdiyne Co_(9)S_(8) S-Scheme heterojunctions Photocatalytic hydrogen evolution

Controllable design of Zn-Ni-P on g-C_3N_4 for efficient photocatalytic hydrogen production

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Chinese Journal of Catalysis 2019年第3期40卷 390-402页

作者： Yanbing Li zhiliang jin Lijun Zhang Kai Fan School of Chemistry and Chemical Engineering North Minzu University Yinchuan 750021 Ningxia China Key Laboratory for Chemical Engineering and Technology State Ethnic Affairs Commission North Minzu University Yinchuan 750021 Ningxia China

Synthesizing a stable and efficient photocatalyst has been the most important research goal up to now. Owing to the dominant performance of g-C3N4 (graphitized carbonitride), an ordered assemble of a composite photocatalyst, Zn-Ni-P@g-C3N4, was successfully designed and controllably prepared for highly efficient photocatalytic H2 evolution. The electron transport routes were successfully adjusted and the H2 evolution was greatly improved. The maximum amount of H2 evolved reached about 531.2 μmol for 5 h over Zn-Ni-P@g-C3N4 photocatalyst with a molar ratio of Zn to Ni of 1:3 under illumination of 5 W LED white light (wavelength 420 nm). The H2 evolution rate was 54.7 times higher than that over pure g-C3N4. Moreover, no obvious reduction in the photocatalytic activity was observed even after 4 cycles of H2 production for 5 h. This synergistically increased effect was confirmed through the results of characterizations such as XRD, TEM, SEM, XPS, N2 adsorption, UV-vis DRS, transient photocurrent, FT-IR, transient fluorescence, and Mott-Schottky studies. These studies showed that the Zn-Ni-P nanoparticles modified on g-C3N4 provide more active sites and improve the efficiency of photogenerated charge separation. In addition, the possible mechanism of photocatalytic H2 production is proposed.

关键词： Zn-Ni-P g-C3N4 H2 production Controllable design Photocatalyst

Mechanochemical preparation and application of graphdiyne coupled with CdSe nanoparticles for efficient photocatalytic hydrogen production

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Chinese Journal of Catalysis 2022年第10期43卷 2708-2719页

作者： Zhaobo Fan Xin Guo Mengxue Yang zhiliang jin School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021NingxiaChina

Graphdiyne(GDY)has attracted considerable attention as a new two-dimensional(2D)carbon hybrid material because of its good conductivity,adjustable electronic structure,and special electron transfer enhancement *** has great potential in the field of photocatalytic water splitting for hydrogen evolution,owing to its unique *** this study,GDY was successfully prepared by the mechanochemical coupling of precursors C_(6)Br_(6) and CaC_(2) using a ball-milling *** prepared GDY,especially its microstructure and composition,was well characterized using different techniques such as X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),Fourier-transform infrared,and Raman characterization *** exploiting the unique two-dimensional(2D)structure and outstanding light absorption properties of GDY,GDY/CdSe 2D/0D heterojunctions were successfully established and applied to photocatalytic hydrogen *** hydrogen evolution activity of GDY/CdSe-20,a type of composite material,reached 6470μmol g^(-1) h^(-1),which is 461 and 40 times higher than that of GDY and CdSe,***,the fine electrical conductivity of GDY enabled rapid and effective transfer of the photogenerated electrons in CdSe into the hydrogen evolution *** transfer path of the photogenerated electrons was studied through XPS with in situ irradiation,and a reasonable mechanism for the hydrogen evolution reaction was *** study provides a feasible approach for the large-scale preparation of GDY and demonstrates the prospects of GDY in the field of photocatalysis.

关键词： Graphdiyne Mechanical ball-milling CaC2 C6Br6 Hydrogen evolution

Construction of CuO-modified zeolitic imidazolate framework-9 for photocatalytic hydrogen evolution

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Chinese Journal of Catalysis 2017年第12期38卷 2056-2066页

作者： Kai Fan zhiliang jin Hong Yuan Hongyan Hu Yingpu Bi School of Chemistry and Chemical Engineering North Minzu University Yinchuan 750021 Ningxia China State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical Physics Chinese Academy of Sciences Lanzhou 730000Gansu China

An efficient CuO‐modified zeolitic imidazolate framework‐9(ZIF‐9)photocatalyst is successfully prepared at room temperature under mild *** is observed that the ZIF‐9/CuO photocatalyst is effective for H2generation under visible light with sacrificial agent *** the CuO is introduced,the photocatalytic properties of ZIF‐9are greatly improved and when the content of CuO is40%,the photocatalytic activity reaches a maximum of78.74μmol *** results from the200–300nm cube structure of ZIF‐9being able to adsorb more dye molecules and the CuO,which connects with ZIF‐9,greatly improving the electronic transmission ***,the interaction between the dye molecule Eosin Y(EY)and the catalyst is also studied by transient fluorescence spectroscopy.A series of characterizations,such as SEM,TEM,XPS,XRD,UV‐vis,FTIR,transient fluorescence and photocurrent,are conducted,and the results are in good agreement with the experimental *** addition,the possible reaction mechanism over EY‐sensitized ZIF‐9/CuO under visible light irradiation is proposed.

关键词： ZIF‐9 CuO Eosin Y Sensitized pathway Hydrogen evolution Reaction optimization

Unique synergistic effects of ZIF-9（Co）-derived cobalt phosphide and CeVO4 heterojunction for efficient hydrogen evolution

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Chinese Journal of Catalysis 2020年第1期41卷 82-94页

作者： Lijun Zhang Xuqiang Hao Junke Li Yuanpeng Wang zhiliang jin School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021NingxiaChina Key Laboratory for Chemical Engineering and Technology State Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021NingxiaChina Ningxia Key Laboratory of Solar Chemical Conversion Technology North Minzu UniversityYinchuan 750021NingxiaChina

The photocatalytic decomposition of water to produce hydrogen is an important process,through which solar energy can be converted to chemical ***-precious metal phosphides have quietly attracted attention as an emerging inexpensive *** this study,we reported that a CoP/CeVO4 hybrid photocatalyst exhibited high hydrogen evolution efficiency owing to EY(eosin Y)sensitization under visible light irradiation for the first time,and the amount of generated hydrogen reached 444.6μmol in 5 *** CoP/CeVO4 nanohybrids were synthesized by a simple chemical precipitation *** coupling of CoP and CeVO4 with ZIF-9 as a precursor could be completed in one *** CeVO4 particles were firmly attached to the surface of the CoP particles to form a"small point"to"big point"*** results of X-ray diffraction,X-ray photoelectron spectroscopy,scanning electron microscopy,EDX,and transmission electron microscopy showed the formation of CoP and CeVO4 nanoparticles and the structure of the *** on a detailed analysis of the Mott-Schottky plot,the UV-vis diffuse reflectance spectra,photocurrent-time(it)curve,Tafel curve,Nyquist curve(EIS),linear volt-ampere curve(LSV),and steady-state fluorescence spectra were *** time-resolved photoluminescence measurements indicated that the reason for the high-efficiency hydrogen evolution of CoP/CeVO4 was that the bands of CoP and CeVO4 were bent due to the existence of the Schottky barrier,and a heterojunction was formed between CoP and CeVO4,which generated an internal electric field and accelerated the charge *** addition,the synergistic effect between CoP and CeVO4 provided a new hydrogen-evolution activity center for each of *** improved carrier separation efficiency and the decrease in the photo-generated recombination rate led to the excellent photocatalytic hydrogen-evolution activity of the CoP/CeVO4 composite *** work provides a new strategy for modulating the el

关键词： Photocatalysis CoP CeVO4 Dye-sensitized Hydrogen production

Tribological properties of M0S_(2) coating for ultra-long wear-life and low coefficient of friction combined with additive g-C3N4 in air

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Friction 2021年第4期9卷 789-801页

作者： Yupeng ZHANG Panpan LI Li JI Xiaohong LIU Hongqi WAN Lei CHEN Hongxuan LI Zhiiiang jin State Key Laboratory of Solid Lubrication Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China School of Chemistry and Chemical Engineering North Minzu UniversityYinchuan 750021China

The solid lubricant M0S_(2) demonstrates excellent lubricating properties,but it spontaneously oxidizes and absorbs moisture in air,and thus results in poor wear resistance and short *** this study,the additive g-C_(3)N_(4)(CN)was successfully combined with M0S_(2) via hydrothermal synthesis as a solid lubricant for the first ***,a low friction coefficient(COF,y=0.031)and ultra-long wear-life of CN/M0S_(2) compared to pure M0S_(2) in air were *** functional groups and good crystallinity of the lubricant material were characterized via Fourier transform infrared(FTIR)spectroscopy and X-ray diffraction(XRD).The formed valence states in CN/M0S_(2) were analyzed via X-ray photoelectron spectroscopy(XPS).The characterized results of the scanning electron microscopy(SEM)and high-resolution transmission electron microscopy(HRTEM)show the morphology and interior crystal phase structure of CN/M0S_(2).From the cross-section analysis,the presence of iron oxide nanoparticles lubricating film is synergistic with CN/M0S_(2) film during the friction process,resulting in its ultra-long *** particular,the friction mechanism of interlayer sliding friction combined with energy storage friction was analyzed and proposed.

关键词： solid lubricant CN/M0S2 friction coefficient(COF) wear-life

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石墨炔基S型异质结构建及平米级光催化产氢

Science China Materials 2024年第2期67卷 493-503页

作者：杨成李小红靳治良 School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion TechnologyKey Laboratory for Chemical Engineering and TechnologyState Ethnic Affairs CommissionNorth Minzu UniversityYinchuan 750021China

石墨炔由于其高载流子迁移率和有序的孔隙结构被认为是一种很有应用前景的光催化材料.本研究通过交叉偶联合成了一种新型球状石墨炔,并与棒状Mn_(0.2)Cd_(0.8)S耦合构建了S型异质结用于光催化析氢.结果表明,Mn_(0.2)Cd_(0.8)S/石墨炔异... 详细信息

石墨炔由于其高载流子迁移率和有序的孔隙结构被认为是一种很有应用前景的光催化材料.本研究通过交叉偶联合成了一种新型球状石墨炔,并与棒状Mn_(0.2)Cd_(0.8)S耦合构建了S型异质结用于光催化析氢.结果表明,Mn_(0.2)Cd_(0.8)S/石墨炔异质结光催化剂表现出优异的光催化活性,产氢性能分别较Mn_(0.2)Cd_(0.8)S和球形石墨炔单体催化剂提升了16.78和613.2倍.同时,该催化剂应用于平米级规模产氢取得较好效果.其优异的光催化活性可归因于石墨炔的独特性能及S-scheme异质结的有效构建.通过紫外光电子能谱、原位辐射X射线光电子能谱、电子顺磁共振能谱、密度泛函理论计算和其他表征技术探究了S-scheme异质结的形成和光催化活性的增强.该工作可为石墨炔的形貌可调性制备以及高效异质结光催化剂的设计和合成提供新参考.

关键词： spherical graphdiyne Mn_(0.2)Cd_(0.8)S DFT S-scheme heterojunction square meter-scale photocatalytic hydrogen production

Ni,Co基硒化物修饰g-C_(3)N_(4)光催化产氢研究

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物理化学学报 2021年第10期37卷 120-134页

作者：靳治良李彦兵郝旭强北方民族大学化学与化学工程学院宁夏太阳能化学转化技术重点实验室国家民委化工技术基础重点实验室银川750021

新型高效的催化剂是突破单体光催化材料载流子低分离和转移效率的重要途径。本文将Ni_(3)Se_(4)和CoSe_(2)纳米粒子锚定在具有良好分散性的g-C_(3)N_(4)纳米片表面,合成了两种新的g-C_(3)N_(4)@Ni_(3)Se_(4)和g-C_(3)N_(4)@CoSe_(2)光... 详细信息

新型高效的催化剂是突破单体光催化材料载流子低分离和转移效率的重要途径。本文将Ni_(3)Se_(4)和CoSe_(2)纳米粒子锚定在具有良好分散性的g-C_(3)N_(4)纳米片表面,合成了两种新的g-C_(3)N_(4)@Ni_(3)Se_(4)和g-C_(3)N_(4)@CoSe_(2)光催化剂并实现了原位光催化析氢。相当严重的载流子的重组导致g-C_(3)N_(4)单体展现了大约只有1.9μmol∙h^(−1)的极差的光催化析氢活性。Ni_(3)Se_(4)和CoSe_(2)纳米颗粒对于加速载流子快速分离和转移的独特作用使得在g-C_(3)N_(4)表面负载Ni_(3)Se_(4)和CoSe_(2)纳米粒子极大地提高了其产氢活性。G-C_(3)N_(4)@Ni_(3)Se_(4)展示了一个大约16.4μmol∙h^(−1)的光催化产氢活性并且g-C_(3)N_(4)@CoSe_(2)展现了一个大约25.6μmol∙h^(−1)的光催化产氢活性,这分别是g-C_(3)N_(4)单体的8倍和13倍。其中,将Ni_(3)Se_(4)和CoSe_(2)与g-C_(3)N_(4)耦合可以显著提高光吸收密度以及扩展光响应范围。激发态EY在g-C_(3)N_(4)@Ni_(3)Se_(4)和g-C_(3)N_(4)@CoSe_(2)存在时比在g-C_(3)N_(4)存在时展现了更低的荧光强度,并且在g-C_(3)N_(4)@Ni_(3)Se_(4)和g-C_(3)N_(4)@CoSe_(2)体系中可观察到最大的电子转移速率。相比g-C_(3)N_(4)@Ni_(3)Se_(4)@FTO和g-C_(3)N_(4)@CoSe_(2)@FTO电极,g-C_(3)N_(4)@@FTO显现了最小的光电流响应密度和最大的电化学,这表明在g-C_(3)N_(4)纳米片表面引入Ni_(3)Se_(4)和CoSe_(2)纳米颗粒增强了光生载流子的分离和转移效率,即基于g-C_(3)N_(4)的金属硒化的合成有效地抑制了光生载流子的复合以及促进了光催化水裂解制氢反应。同时,吸收带边的红移有效地降低了光激电子从价带到导带跃迁的阈值。此外,g-C_(3)N_(4)@Ni_(3)Se_(4)和g-C_(3)N_(4)@CoSe_(2)复合催化剂的zeta电位比g-C_(3)N_(4)的更负,说明样品表面对质子增强的吸附。并且密度泛函理论结果表明:g-C_(3)N_(4)中N位点对H的吸附能为−0.22 eV,还发现氢原子更倾向于吸附在两个硒原子的桥位点上形成Se―H―Se键,并且吸附能为1.53 eV。所有对样品进行的透射电子显微镜(TEM)、扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、X射线衍射(XRD)、紫外可见漫反射光谱(UV-Vis-DRS)、瞬态光电流、傅立叶变换红外光谱(FT-IR)等相关表征都展示了彼此匹配的结果。

关键词： Ni3Se4 CoSe2 g-C_(3)N_(4) 析氢