氧空位锚定铂单原子增强氢溢流促进逆水煤气变换反应
Pt single atoms in oxygen vacancies boost reverse water-gas shift reaction by enhancing hydrogen spillover
康鑫 1刘健聪 1谢颖 1王东旭 1刘骐珲 1于鹏 2田春贵 1付宏刚1
作者信息
- 1. Key Laboratory of Functional Inorganic Material Chemistry,Ministry of Education,Heilongjiang University,Harbin 150080,China
- 2. Key Laboratory for Photonic and Electronic Bandgap Materials,Ministry of Education,School of Physics and Electronic Engineering,Harbin Normal University,Harbin 150025,China
- 折叠
摘要
构建单原子催化剂(SACs)和载体氧空位(Ov)的协同催化对于提高CO2加氢催化效率至关重要,但同时也面临着诸多挑战.在本研究中,我们开发了一种胺分子辅助原位锚定策略,通过控制胺分子与铂(Pt)物种和TiO2-x之间的相互作用,成功实现Pt单原子在TiO2-x上的有效分散与稳定.直接证据表明,Pt SACs嵌入Ov中形成Ptδ+-Ov-Ti3+结构,并展现出强金属-载体相互作用,这不仅抑制了高温还原过程中Pt SACs的烧结,还增强了氢溢流过程,促进了更多Ov位点的形成.在逆水煤气变换(RWGS)反应中,增加的Ov位点数量可以促进CO2的吸附,而Pt SACs则有效提升了氢的活化和溢流.二者的协同作用显著提高了材料的催化性能,是其在330℃下具有高达9289 h-1的转化频率(TOF)和超过200小时的高稳定性,超越了TiO2-x上负载Pt团簇和纳米颗粒催化剂.本工作为可控制备具有单原子和Ov的协同催化剂开辟了一条新的途径.
Abstract
The construction of synergistic catalysis of single atom catalysts(SACs)and oxygen vacancies(Ov)on supports is crucial for the enhancement of heterogeneous catalytic efficiency,yet presents considerable challenges.Herein,we have developed an amine-molecule-assisted in-situ anchoring strategy that effectively stabilizes Pt SACs on Ov sites of reduced TiO2(TiO2-x)by controlling the interaction of amine with Pt species and TiO2-x.Direct evidence indicates that Pt SACs are anchored on the Ov with forming Pts+-Ov-Ti3+sites and strong metal-support interaction,which not only prevents the sintering of Pt SACs under high-temperature reduction treatments,but also enhances the hydrogen spil-lover process to facilitate the formation of more Ov sites.During the reverse water-gas shift(RWGS)reaction,the en-hanced amount of Ov sites can increase CO2 adsorption,while the Pt SACs can efficiently promote the activation and spil-lover of hydrogen.Their combined synergistic effects greatly improve its catalytic performance with a high turnover fre-quency(TOF)of 9289 h-1 at 330℃ and notable stability for over 200 h,surpassing those of Pt clusters and nanoparticles on TiO2-x.This work provides a new avenue for the con-trollable synthesis of synergistic catalysts with SACs and Ov,significantly advancing catalytic efficiency.
关键词
Pt single atoms/oxygen vacancies/TiO2/reverse water-gas shift reaction/hydrogen spilloverKey words
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出版年
2024
NETL
NSTL
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