摘要
Thermochemical two-step CO_(2) splitting is a potential approach that fixes the sustainable resource into transportable liquid fuels.However,the harsh CO_(2) splitting conditions,the limited oxygen release kinetics and capacity of metal oxides block further promoted the CO yield and solar-to-fuel energy efficiency.Here,we propose a different carbon cycle assisted by Ni/La_(2)O_(3) via coupling methane decomposition with thermochemical CO_(2) splitting,replacing conventional metal oxides cycle.Superior performance was demonstrated with methane conversion reached around 94%with almost pure H_(2) generation.Encouragingly,CO_(2) conversion of 98%and CO yield of 6.9 mmol g^(-1) derived from CO_(2) were achieved,with peak CO evolution rate(402 mL min^(-1) g^(-1))of orders of magnitude higher than that in metal oxide process and outstanding thermodynamic solar-to-fuel energy efficiency(55.5%vs.18.5%).This was relevant to the synergistic activation of La_(2)O_(3) and Ni for CO_(2) in carbon cycle,thus improving CO_(2) splitting reaction with carbon species.
基金
supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100)
the National Key R&D Program of China(2016YFA0202-801)
the National Natural Science Foundation of China(NSFC)grants(21676269,21706254,21878283,22022814)
the Dalian Institute of Chemical Physics,CAS(DICP I201916)。
作者简介
Yu Kang,contributed equally to this work;Yujia Han,contributed equally to this work;Cong Wei,contributed equally to this work;Corresponding authors:Ming Tian,E-mail addresses:tm1982@dicp.ac.cn;Corresponding authors:Riguang Zhang,E-mail addresses:zhangriguang@tyut.edu.cn;Corresponding authors:Xiaodong Wang,E-mail addresses:xdwang@dicp.ac.cn。
