铁掺杂氮化碳/BiVO_(4)构建Z型光催化全解水  

Iron-doped C3N4/BiVO_(4) as a Z-scheme Photocatalyst System for Water Splitting

作　　者：刘智焬 戚荣杰 罗皓霖 叶朕 江治[1] 上官文峰[1] LIU Zhi-xi;QI Rong-jie;LUO Hao-in;YE Zhen;JIANG Zhi;SHANGGUAN Wen-feng(Research Center for Combustion and Environmental Technology,Shanghai Jiao Tong University,Shanghai 200240,China)

机构地区：[1]上海交通大学机械与动力工程学院,上海200240

出　　处：《分子催化（中英文）》2024年第2期112-120,I0001,I0002,共11页Journal of Molecular Catalysis(China)

基　　金：国家自然科学基金项目(No.21872093);国家重点研发计划项目(No.2018YFB1502001)。

摘　　要：采用气相挥发法在聚合物氮化碳(PCN)结构中引入了适量的铁(Fe)掺杂组分,成功制备出具有可调Fe掺杂浓度的PCN半导体光催化剂,其中0.55%(w) Fe掺杂的PCN析氢催化活性(410μmol·h^(-1))为原始PCN的2.6倍并通过XRD、UV-Vis、PL、XPS、SEM等表征阐明了Fe掺杂对PCN的影响和作用机理.同时调控钒酸铋的生长环境(配合剂、水热时间、pH)合成了具备不同形貌的钒酸铋(BiVO4),进一步成功合成了暴露{010}和{-121}晶面的十面体BiVO_(4).Z型体系中还原和氧化过程分离,可以在不同催化剂上分别进行氧化还原反应,能够有效抑制逆反应的发生,同时扩宽光催化材料的设计和选择的可能性.以PCN作为产氢端催化剂,十面体BiVO_(4)作为产氧端催化剂,以Fe^(3+)/Fe^(2+)作为离子对构建了Z型体系实现了光催化全解水.其中0.55%Fe掺杂的PCN-Fe/BiVO_(4)表现出了更优异的光催化活性,全解水的产氢性能比未改性的PCN/BiVO_(4)提升近一倍,进一步验证了气相挥发法掺杂Fe改性策略的有效性.这种基于催化剂(氮化碳)性质的掺杂改性方法对于催化剂的优化和设计以及构建Z型光催化全解水体系的探索具备一定的借鉴意义.PCN semiconductor photocatalysts with adjustable Fe doping concentration were successfully prepared using the gas-phase volatilization method to introduce an appropriate amount of iron(Fe)doping components into the polymer carbon nitride(PCN)structure.The 0.55%(mass fraction)Fe-doped PCN showed a 2.6 times higher photocatalytic activity(410μmol∙h^(-1))compared to the pristine PCN.The characterization of XRD,UV-Vis,PL,XPS,and SEM was used to elucidate the mechanism of Fe doping on PCN.The growth environment of bismuth vanadate was adjusted to synthesize the decahedral BiVO_(4) with exposed{010}and{-121}crystal planes was successfully synthesized.The Z-type system separates reduction and oxidation processes,enabling redox reactions to occur independently on distinct catalysts.This effectively inhibits the occurrence of the inverse reaction and broadens the possibilities for designing and selecting photocatalytic materials.The Z-scheme system was achieved by utilizing PCN as the catalyst for HER,decahedral BiVO4 as the catalyst for OER,and Fe^(3+)/Fe^(2+)as the ion pair.The PCN-Fe/BiVO_(4) doped with 0.55%Fe showcased the highest level of photocatalytic activity.The result was nearly twice as high as the unmodified PCN/BiVO_(4).This finding affirms the effectiveness of the Fe-doped modification method utilizing the gas-phase volatilization technique.

关 键 词：氮化碳 铁掺杂 钒酸铋 Z型体系 光催化 

分 类 号：O643.32[理学—物理化学]