文献类型：期刊文献

英文题名：Synergistic Effect between Oxygen Vacancy and Bronsted Acid Sites Boosting Efficient Hydrogenolysis of Esters to Alkanes

作者：Cao, Xincheng[1,2,3,4] Jia, Shuya[5] Zhang, Yao[2,3,4] Long, Feng[2,3,4] Chen, Yuwei[6] Liu, Peng[2,3,4] Zhang, Xiaolei[5] Xu, Junming[2,3,4] Jiang, Jianchun[1,2,3,4]

第一作者：Cao, Xincheng

通信作者：Jiang, JC[1];Liu, P[2];Xu, JM[2];Jiang, JC[2];Liu, P[3];Xu, JM[3];Jiang, JC[3];Liu, P[4];Xu, JM[4];Jiang, JC[4]

机构：[1]Huaqiao Univ, Acad Adv Carbon Convers Technol, Coll Chem Engn, Xiamen 361021, Fujian, Peoples R China;[2]Chinese Acad Forestry, Inst Chem Ind Forest Prod, Key Lab Biomass Energy & Mat, SAF, Nanjing 210042, Jiangsu, Peoples R China;[3]Chinese Acad Forestry, Inst Chem Ind Forest Prod, Natl Engn Lab Biomass Chem Utilizat, SAF, Nanjing 210042, Peoples R China;[4]Chinese Acad Forestry, Inst Chem Ind Forest Prod, Key & Open Lab Forest Chem Engn, SAF, Nanjing 210042, Peoples R China;[5]Univ Strathclyde, Dept Chem & Proc Engn, Glasgow G1 1XJ, Scotland;[6]Yancheng Inst Technol, Yancheng 224051, Peoples R China

年份：2025

卷号：13

期号：16

起止页码：6010-6020

外文期刊名：ACS SUSTAINABLE CHEMISTRY & ENGINEERING

收录：;EI(收录号：20251618269250);Scopus(收录号：2-s2.0-105002842288);WOS:【SCI-EXPANDED(收录号:WOS:001470154000001)】；

基金：This work was supported by the National Natural Science Foundation of China (32301548), the Postdoctoral Fellowship Program of CPSF under Grant Number GZC20230878, and the Young Talent Promotion Project of Jiangsu Association for Science and Technology (JSTJ-2023-XH019).

语种：英文

外文关键词：identifying active sites; synergistic effect; hydrodeoxygenation; biomass-derived esters

摘要：Fundamental knowledge of the active site requirements for the activation of C-O bonds on heterogeneous catalysts is essential for the design of efficient hydrodeoxygenation catalysts. Pt-WOx (x < 3) catalysts have shown activity and selectivity for the C-O bond breaking of various biomass-derived oxygenates. Yet, the nature of the active sites and the structure-performance relationship have not been well understood because of the intimate coupling of multiple sites. Here, we construct a hybrid catalyst with integrated defective tungsten oxide (e.g., WO2.72) and Pt/C to investigate the role of multiple sites (e.g., metal sites, Bronsted acid, and oxygen vacancy) that are active toward the hydrogenolysis of esters to alkanes in Pt-WOx catalysts. Experimental and theoretical results suggest that oxygen vacancies derived from the defective tungsten oxide (WOx) supply coordinatively unsaturated sites to adsorb and activate the oxygen atom of the carbonyl group of esters, while Pt metal provides an active hydrogen atom for this process. More importantly, it is found that the hydroxyl derived from W-OH in WOx, as a typical Bronsted acid site, can contribute to the adsorption and activation of the C-O bond of esters. The synergistic effect of oxygen vacancies and Bronsted acid sites results in a remarkably efficient acyl C-O bond cleavage of esters, which boosts the hydrodeoxygenation of esters under mild conditions (T <= 200 degrees C). These insights into the structure-performance relationships offer rational methods for designing efficient catalysts for low-temperature hydrodeoxygenation of biomass-derived esters.