Oxygen vacancies-elusive but common catalytic key defects for thermal upgrading of CO_(2) to CH_(4),CO and CH_(3)OH  

作　　者：Sebastian Cisneros Jabor Rabeah 

机构地区：[1]State Key Laboratory of Low Carbon Catalysis and Carbon Dioxide Utilization,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,730000 Lanzhou,Gansu,China [2]Leibniz-Institut für Katalyse,Albert-Einstein-Str.29A,18059 Rostock,Germany

出　　处：《Journal of Energy Chemistry》2025年第3期852-892,共41页能源化学(英文版)

基　　金：the financial support from the European Commission through the H2020-MSCA-RISE-2020 BIOALL project(Grant Agreement: 101008058)。

摘　　要：Single carbon products(C1 compounds) are simple but important chemicals in the road towards energy transition.Catalytic conversion of CO_(2) with H_(2)(desirably renewable) can be performed over reducible oxides supporting transition metals to obtain products such as CH_(4),CO and MeOH.Oxygen vacancies(O-vacancies),which are inherent defects of reducible metal oxides,play an enormous role in driving the catalytic performance(activity,selectivity,stability) for the desired reactions.Yet,the assessment of O-defects at realistic conditions is often complex.Only few techniques can provide direct evidence for their existence and influence in CO_(2) activation.Among them,electron paramagnetic spectroscopy(EPR),Raman spectroscopy,scanning probe microscopies(SPM) and environmental transmission electron microscopy(ETEM) are nowadays the most informative.In most cases,however,the measurements require reaction conditions far away from CO_(2) valorization applications.Although great efforts have been fruitful in explaining and demonstrating the huge importance of O-vacancies in CO_(2) catalysis,still ambiguous or erroneous interpretations about structure-function correlations involving O-vacancies are found in literature,especially,when information is not properly gathered,e.g.,by O 1s ex-situ X-ray photon spectroscopy(XPS).Moreover,despite the recognized importance of O-vacancies for CO_(2) valorization,critical literature compilations about their effects in thermal processes are scarce.Herein,we attempt to contribute in closing this gap by integrally encompassing representative investigations on the thermo-catalytic production of CH_(4),CO and MeOH.Particularly,we emphasize on the proper selection of assessment tools(direct/indirect) to unambiguously establish structure-function relationships to design optimized O-defective catalysts for the targeted compounds.

关 键 词：Oxygen vacancy CO_(2) Methane Carbon monoxide METHANOL 

分 类 号：O643.36[理学—物理化学]