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投稿时间:2022-12-02 修订日期:2022-12-07 录用日期:2022-12-12 网络发布日期:2023-03-17
投稿时间:2022-12-02 修订日期:2022-12-07 录用日期:2022-12-12 网络发布日期:2023-03-17
中文摘要: 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-CeO2)为载体,负载非贵金属Co制备催化剂Co/P-CeO2,该催化剂展示了优异的可见光催化氨硼烷(NH3BH3)水解制氢活性。当CeO2与NaH2PO2的摩尔比为1.6时(P-CeO2-1.6),Co/P-CeO2-1.6水解NH3BH3反应的转化频率(TOF)值为81.83 min-1,与Co/CeO2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NH3BH3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。
Abstract: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-CeO2 with rich oxygen vacancies and P doping by sodium hypophosphite (NaH2PO2) heat treatment was prepared to support metal Co to achieve the catalyst Co/P-CeO2. The catalyst exhibites excellent catalytic performance for hydrogen evolution from ammonia borane (NH3BH3) under visible irradiation. When the molar ratio of CeO2 and NaH2PO2 is 1.6, turnover frequency (TOF) of Co/P-CeO2-1.6 is 81.83 min-1, which rises up 25.5% compared with that of CeO2. Additionally, Co/P-CeO2-1.6 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 NH3BH3, but also paves the way for designing high performance catalyst by element doping for photocatalytic reactions.
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基金项目: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
引用文本:
宋瑾,吴凤龙.P掺杂CeO2纳米棒负载Co光催化氨硼烷水解产氢[J].有色金属(冶炼部分),2023(4):67-76.
SONG Jin,WU Feng-long.P Doped CeO2 Nanorods Supported Co for Photocatalytic Hydrogen Evolution from Ammonia Borane[J].Nonferrous Metals (Extractive Metallurgy),2023(4):67-76.
宋瑾,吴凤龙.P掺杂CeO2纳米棒负载Co光催化氨硼烷水解产氢[J].有色金属(冶炼部分),2023(4):67-76.
SONG Jin,WU Feng-long.P Doped CeO2 Nanorods Supported Co for Photocatalytic Hydrogen Evolution from Ammonia Borane[J].Nonferrous Metals (Extractive Metallurgy),2023(4):67-76.

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