P掺杂CeO_(2)纳米棒负载Co光催化氨硼烷水解产氢  

P Doped CeO_(2) Nanorods Supported Co for Photocatalytic Hydrogen Evolution from Ammonia Borane

作　　者：宋瑾[1,2] 吴凤龙 SONG Jin;WU Feng-long(Functional Materials Laboratory,Hetao College,Bayannur 015000,Inner Mongolia,China;Development of Ecology and Resource Engineering,Hetao College,Bayannur 015000,Inner Mongolia,China)

机构地区：[1]河套学院功能材料实验室,内蒙古巴彦淖尔015000 [2]河套学院生态与资源工程系,内蒙古巴彦淖尔015000

出　　处：《有色金属（冶炼部分）》2023年第4期67-76,共10页Nonferrous Metals（Extractive Metallurgy)

基　　金：国家自然科学基金资助项目(52161038);内蒙古自治区自然科学基金资助项目(2020MS02021,2022MS05012);内蒙古自治区人才开发基金资助项目(内人社办发[2022]110号);内蒙古自治区高等学校青年科技英才支持计划项目(NJYT23033)。

摘　　要：载体光生载流子的分离效率是影响负载型催化剂活性的重要因素。表面工程是调控载体表面结构、提高催化剂光生载流子分离效率的常见方法。以经过次磷酸钠处理后在表面同时形成氧缺陷与P元素掺杂的二氧化铈(P-CeO_(2))为载体,负载非贵金属Co制备催化剂Co P-CeO_(2),该催化剂展示了优异的可见光催化氨硼烷(NH_(3) BH_(3))水解制氢活性。当CeO_(2)与NaH_(2)PO_(2)摩尔比为1.6时(P-CeO_(2)-1.6),Co P-CeO_(2)-1.6水解NH_(3) BH_(3)反应的转化频率(TOF)值为81.83 min^(-1),与Co CeO_(2)相比活性提高了25.5%,并且具有较好的循环活性。系统表征发现,催化剂活性提高的原因是氧缺陷与P元素掺杂的协同作用,载体在可见区的吸收明显拓宽(吸收边为470 nm),带隙变小(2.55 eV),光生载流子分离效率显著提高。本研究不仅设计合成了高效的光催化NH_(3) BH_(3)水解催化剂,同时为利用元素掺杂制备高效光活性催化剂提供借鉴。The separation efficiency of photogenerated carrier on supports is important factor for activity of support-catalyst.Surface engineering is a common method to improve the separation efficiency of catalysts by modification the surface electronic structure.The P-CeO_(2) with rich oxygen vacancies and P doping by sodium hypophosphite(NaH_(2)PO_(2))heat treatment was prepared to support metal Co to achieve the catalyst Co P-CeO_(2).The catalyst exhibites excellent catalytic performance for hydrogen evolution from ammonia borane(NH_(3) BH_(3))under visible irradiation.When the molar ratio of CeO_(2) and NaH_(2)PO_(2) is 1.6,turnover frequency(TOF)of Co P-CeO_(2)-1.6 is 81.83 min^(-1),which rises up 25.5%compared with that of CeO_(2).Additionally,Co P-CeO_(2)-1.6 also exhibits good cyclic stability.Advanced characterization shows the enhanced activity is ascribed to synergistic effect of oxygen vacancies and P doping,leading to extended absorption edge(470 nm),narrowed band gap(2.25 eV)and higher separation efficiency of photogenerated carrier.This work not only provides an efficient catalyst for hydrogen evolution from NH_(3) BH_(3),but also paves the way for designing high performance catalyst by element doping for photocatalytic reactions.

关 键 词：光生载流子 协同作用 氨硼烷 P掺杂 

分 类 号：TB34[一般工业技术—材料科学与工程] O643.36[理学—物理化学]