摘要
调控金属活性位点的电子结构来发展高活性的选择性加氢反应催化剂对于可持续有机合成非常重要.但时至今日,这仍然是非常具有挑战性的课题.在本文中,我们将具有电子结构调节特性的超细PtRu合金纳米颗粒负载在CdS纳米棒上,成功构建了PtRu/CdS复合催化剂并研究了其光催化芳香族硝基化合物氢化还原性能.我们发现当以水为质子源时,所得复合催化剂表现出高效的光催化加氢活性.超快光谱研究和密度泛函理论计算揭示了合金的形成促进了光生载流子的分离并降低了氢化还原反应中决速步的能垒,从而显著提高了加氢活性.本研究通过合金化效应调节助催化剂的电子结构,为高活性助催化剂/光催化剂体系的理性设计开辟了一条新途径.
Regulating the electronic structure of metal sites to develop high-performance catalysts for selective hydrogenation reactions is very important for sustainable organic synthesis, yet still challenging. Herein, we adopt a facile method to rationally design an ultrafine PtRu alloy cocatalyst on CdS nanorods(PtRu/CdS) for the efficient photocatalytic hydrogenation reaction with water as a proton source. The ultrafast transient absorption spectroscopy studies uncover that alloying promotes the separation of photoexcited carriers,and density functional theory calculations demonstrate that alloying reduces the energy barrier of the rate-determining step, thus enhancing the hydrogenation activity. This work opens a new avenue to rationally design highly-active metalmodified photocatalysts via modulating electronic structures of co-catalysts.
作者
施曼曼
罗点
吴鹏
沈娅蓉
魏杰顶
郭赛雅
陆洲
黄玉成
倪永红
Manman Shi;Dian Luo;Peng Wu;Yarong Shen;Jieding Wei;Saiya Guo;Zhou Lu;Yucheng Huang;Yonghong Ni(College of Chemistry and Materials Science,Key Laboratory of Functional Molecular Solids,Ministry of Education,Anhui Laboratory of Molecule-Based Materials,Anhui Key Laboratory of Functional Molecular Solids,Anhui Normal University,Wuhu 241002,China;School of Physics and Electronic Information,Anhui Normal University,Wuhu 241002,China)
基金
supported by the University Annual Scientific Research Plan of Anhui Province (2022AH010013)。
