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In-situ polymerization induced atomically dispersed manganese sites as cocatalyst for CO2 photoreduction into synthesis gas
Nano Energy ( IF 16.8 ) Pub Date : 2020-06-29 , DOI: 10.1016/j.nanoen.2020.105059
Jia Yang , Zhiyuan Wang , Jianchao Jiang , Wenxing Chen , Fan Liao , Xiao Ge , Xiao Zhou , Min Chen , Ruilong Li , Zhenggang Xue , Gang Wang , Xuezhi Duan , Guoqing Zhang , Yang-Gang Wang , Yuen Wu

Developing highly-active single atom catalyst to realize visible light driven photocatalytic CO2 reduction into value-added chemicals is an appealing route toward utilizing CO2 as the only carbon source for a sustainable future. Herein, we have successfully synthesized the atomically dispersed manganese sites in nitrogen doped carbon via an in-situ polymerization approach. The in-situ oxidative polymerization of pyrrole monomer directly catalyzed by manganese dioxide could extract the Mn atoms from MnO2 and stabilize them within the as-generated polymer skeleton in one step. After high-temperature pyrolysis, atomically dispersed Mn sites are obtained, firmly and homogeneously anchored by the as-generated N-doped carbon support. The as obtained catalyst can act as cocatalyst to realize photocatalytic CO2 reduction to produce synthesis gas under visible light using [Ru(bpy)3]Cl2 (bpy: 2,2′-bipyridine) as photosensitizer and triethanolamine as sacrifacial agent, with gas evolution rate of CO 1470 μmol/h/g, H2 1310 μmol/h/g and tunable CO/H2 ratio from 1.12 to 0.43. Our approach is versatile to prepare a variety of morphology-controllable single atom catalysts from metal oxides for important industrial applications.



中文翻译:

原位聚合诱导原子分散的锰位点作为CO 2光还原成合成气的助催化剂

开发高活性单原子催化剂以实现将可见光驱动的光催化CO 2还原为增值化学品,是利用CO 2作为可持续发展的唯一碳源的诱人途径。在这里,我们已经成功地通过原位聚合方法在氮掺杂碳中合成了原子分散的锰位点。二氧化锰直接催化吡咯单体的原位氧化聚合可以从MnO 2中提取Mn原子。一步将它们稳定在生成的聚合物骨架中。高温热解后,获得原子分散的Mn位点,并牢固地,均匀地固定在刚生成的N掺杂碳载体上。所获得的催化剂可以用作助催化剂,以[Ru(bpy)3 ] Cl 2(bpy:2,2'-联吡啶)为光敏剂,以三乙醇胺为牺牲剂,在可见光下实现光催化CO 2还原,产生合成气。 CO 1470μmol/ h / g,H 2 1310μmol/ h / g和可调CO / H 2的气体逸出速率比从1.12到0.43。我们的方法适用于从重要工业应用的金属氧化物制备各种形态可控的单原子催化剂。

更新日期:2020-06-29
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