文献类型：期刊文献

中文题名：Pd single-atom monolithic catalyst: Functional 3D structure and unique chemical selectivity in hydrogenation reaction

英文题名：Pd单原子整体催化剂:功能化的三维结构和优异的化学加氢选择性

作者：Zedong Zhang[1];Min Zhou[2];Yuanjun Chen[1];Shoujie Liu[3];Haifeng Wang[2];Jian Zhang[1];Shufang Ji[1];Dingsheng Wang[1];Yadong Li[1]

机构：[1]Department of Chemistry,Tsinghua University,Beijing 100084,China;[2]Key Laboratory for Advanced Materials,Centre for Computational Chemistry and Research Institute of Industrial Catalysis,East China University of Science and Technology,Shanghai 200237,China;[3]Chemistry and Chemical Engineering of Guangdong Laboratory,Shantou 515063,China

年份：2021

卷号：64

期号：8

起止页码：1919

中文期刊名：Science China Materials

外文期刊名：中国科学（材料科学（英文版）

收录：Scopus;CSCD:【CSCD2021_2022】；PubMed;

基金：This work was supported by the National Key R&D Program of China (2018YFA0702003), the National Natural Science Foundation of China (21890383, 21671117, 21871159 and 21901135), the National Postdoctoral Program for Innovative Talents (BX20180160), and the China Postdoctoral Science Foundation (2018M640113). We thank the BL14W1 station in Shanghai Synchrotron Radiation Facility (SSRF) and 1W1B station for XAFS measurement in Beijing Synchrotron Radiation Facility (BSRF).

语种：英文

中文关键词：single-atom;monolithic catalyst;isolated site;hydrogenation reaction

外文关键词：单原子催化剂;整体型;可重复使用性;氢化反应;整体催化剂;选择性加氢;回收循环;三维结构;

摘要：Regulating the selectivity of catalysts in selective hydrogenation reactions at the atomic level is highly desirable but remains a grand challenge. Here we report a simple and practical strategy to synthesize a monolithic single-atom catalyst(SAC) with isolated Pd atoms supported on bulk nitrogen-doped carbon foams(Pd-SAs/CNF). Moreover, we demonstrate that the single-atom Pd sites with unique electronic structure endow Pd-SAs/CNF with an isolated site effect, leading to excellent activity and selectivity in 4-nitrophenylacetylene semi-hydrogenation reaction. In addition, benefiting from the great integrity and excellent mechanical strength, monolithic Pd-SAs/CNF catalyst is easy to separate from the reaction system for conducting the subsequent recycling. The cyclic test demonstrates the excellent reusability and stability of monolithic Pd-SAs/CNF catalyst.The discovery of isolated site effect provides a new approach to design highly selective catalysts. And the development of monolithic SACs provides new opportunities to advance the practical applications of single-atom catalysts.
原子级别调控催化剂在选择性加氢反应中的选择性是一个巨大的挑战.在本文中,我们报告了一种简单实用的策略,用于合成Pd单原子负载在氮掺杂碳纳米泡沫(Pd-SAs/CNF)上的整体型单原子催化剂.此外,我们证明独特电子结构的单原子Pd位点使得PdSAs/CNF产生孤立位点效应,进而导致在4-硝基苯基乙炔半氢化反应中具有出色的活性和选择性.此外,得益于较高的完整性和良好的机械强度,整体型Pd-SAs/CNF催化剂易与反应体系分离,进一步有利于回收循环利用.循环测试表明,整体型Pd-SAs/CNF催化剂具有优异的可重复使用性和稳定性.孤立位点效应的发现为设计高选择性催化剂提供了一种新方法.整体式单原子催化剂的研究为推进单原子催化剂的实际应用提供了新的机会.