Synthesis of methanol via CO_(2) hydrogenation catalyzed by La_(2)O_(2)CO_(3)/Cu catalysts  

作  者:Jun He Chenglong Yu Zhijuan Zhao Bo Guan Bin Zhang Yanru Zhang Longbo Zhang Yanyan Wang Ying Wang Yahui Wu Jia Guo Yang Li Tianbin Wu Qingli Qian Hongxing Wang Buxing Han 

机构地区:[1]Beijing National Laboratory for Molecular Sciences,Key Laboratory of Colloid and Interface and Thermodynamics,Center for Carbon Neutral Chemistry,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China [2]College of Chemical Engineering and Materials Science,Tianjin University of Science and Technology,Tianjin 300457,China [3]School of Chemical Sciences,University of Chinese Academy of Sciences,Beijing 100049,China [4]Center for Physicochemical Analysis Measurements,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190,China [5]Shanghai Key Laboratory of Green Chemistry and Chemical Processes,State Key Laboratory of Petroleum Molecular and Process Engineering,School of Chemistry and Molecular Engineering,East China Normal University,Shanghai 200062,China

出  处:《Nano Research》2025年第2期153-163,共11页纳米研究(英文版)

基  金:The work was financially supported by the National Key Research and Development Program of China(No.2024YFE0206500);the National Science Foundation of China(Nos.22033009,22072156,22073104 and 22121002).

摘  要:The development of efficient Cu-based heterogeneous catalysts for CO_(2) hydrogenation to methanol has been an appealing subject.Inspired by the concept of inverse catalysts,a series of La_(2)O_(2)CO_(3)/Cu nanorod composites with varying Cu contents(denoted as LOC/Cu-x,where x stands for the mass ratio of La and Cu in the catalysts)were prepared by combining coprecipitation and calcination processes.Remarkable composition-dependence of catalytic activity and selectivity were observed when different LOC/Cu-x(x=0.1,0.2,0.5,1,3 and 5)were used to catalyze the CO_(2) hydrogenation.The predominant product shifted from methane to methanol with the increasing Cu content.The highest reaction rate(13.3 mmol·gCu^(-1)·h^(-1))and methanol selectivity(85.5%)were achieved when LOC/Cu-1 was tested at 200℃.The LOC was not active for the reaction,while the Cu itself displayed poor catalytic performance.The Cu–LOC interactions significantly affected the nature of the catalysts,including mutual electron transfer,crystal structure,morphology,porosity,surface Cu valence and capability of adsorbing the reactant gases,etc.,which account for the outstanding behavior of the LOC/Cu-1 catalyst.This work provides a new strategy for the design and optimization of Cu-based catalysts.

关 键 词:CO_(2)hydrogenation METHANOL heterogeneous catalysts Cu-La_(2)O_(2)CO_(3)(LOC)interaction 

分 类 号:O64[理学—物理化学]

 

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