Co-thermal in-situ reduction of inorganic carbonates to reduce carbon-dioxide emission

作     者：Zhen Xue Jingyi Guo Shasha Wu Wenfu Xie Yujing Fu Xiaojie Zhao Kui Fan Ming Xu Hong Yan Mingfei Shao Xue Duan Zhen Xue;Jingyi Guo;Shasha Wu;Wenfu Xie;Yujing Fu;Xiaojie Zhao;Kui Fan;Ming Xu;Hong Yan;Mingfei Shao;Xue Duan

作者机构：State Key Laboratory of Chemical Resource EngineeringBeijing University of Chemical TechnologyBeijing 100029China 

出 版 物：《Science China Chemistry》 (中国科学（化学英文版）)

年 卷 期：2023年第66卷第4期

页      面：1201-1210页

核心收录：

学科分类：07[理学] 070304[理学-物理化学(含∶化学物理)] 0703[理学-化学] 070301[理学-无机化学] 0702[理学-物理学] 

基　　金：supported by the National Natural Science Foundation of China(21922501,21871021,22102007) the Fundamental Research Funds for the Central Universities(buctrc202112)。 

主　　题：inorganic carbonate co-thermal in-situ reduction carbon dioxide emission reduction carbon monoxide 

摘      要：Thermal decomposition of inorganic metal carbonates is the main path to prepare metal oxides;nonetheless,it is always accompanied by the emission of large amounts of CO_(2) as one of the gas products.This study reports a concept of co-thermal insitu reduction of inorganic carbonates by using the energy released by carbonate decomposition under pure hydrogen atmosphere,which reduces the decarboxylation temperature and significantly inhibits the CO_(2) emissions.A combination of hydrogen–deuterium exchange,isotope experiment,and density functional theory calculations demonstrates that the CO results from the selective cleavage of Ca–O bonds at the surface of CaCO_(3) via the direct hydrogenation mechanism at relatively low temperature.However,it undergoes the reverse water–gas shift reaction path at high temperature,i.e.,CO being produced by the reduction of CO_(2) released by the decomposition of carbonates.This study sheds light on the potential of green hydrogen technology for inorganic carbonate valorization toward high value-added products,which can facilitate the large-scale industrial applications.