The Ga-promoted Ni/CeO2 catalysts for dry reforming of methane with high stability induced by the enhanced CO2 activation

The Ga-promoted Ni/CeO2 catalysts for dry reforming of methane with high stability induced by the enhanced CO2 activation
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Ga促进的Ni/CeO2催化剂用于甲烷干重整,通过增强CO2活化而具有高稳定性

DOI:
10.1016/j.mcat.2022.112577
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发表时间:
2022-09
影响因子:
4.6
通讯作者:
Zhikun Peng
Zhikun Peng
中科院分区:
化学2区
文献类型:
--
作者:
Yuanyuan Bai;Kaihang Sun;Jinwei Wu;Yizhuo Han;Shufang Zhao;Young Dok Kim;Yujia Liu;Jie Gao;Zhongyi Liu;Zhikun Peng

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• 通过Ga掺杂成功调节Ni/CeO 2 催化剂的碱度,增强了CO 2 的吸附和活化能力。 • Ga掺杂量为3wt.%的Ni/CeO 2 催化剂具有更多的碱性位点,可以产生足够的氧物种来消除反应中的焦炭,并表现出高度的稳定性。镍基催化剂在甲烷干重整反应中表现出较高的活性,但存在严重的积炭和失活问题。合成了一系列不同Ga含量促进的CeO 2 负载Ni催化剂,并调节了催化剂的碱性位点。 3 wt% Ga掺杂的Ni/CeO 2 催化剂表现出最高的活性(X CH 4 = 74%和X CO 2 = 88%)和稳定性,反应35小时后H 2 /CO比为0.94,没有任何碳沉积。 CH 4 -CO 2 -CH 4 脉冲实验表明Ga的掺杂可以产生足够的氧物种来消除积碳并保持催化活性。优异的活性和更好的稳定性可归因于Ga的引入增强了催化剂碱性位点上的CO 2 吸附和活化。这些结果为Ni/CeO 2 催化体系中Ga调节的碱性位点与催化剂稳定性之间的关系提供了基本的了解。 Ga的掺杂成功调节了Ni/CeO 2 催化剂的碱度,促进了CO 2 的吸附和活化,提高了催化活性和稳定性。
• The basicity of the Ni/CeO 2 catalyst was successfully adjusted by Ga doping and enhanced the adsorption and activation capacity of CO 2 . • The Ni/CeO 2 catalyst with 3 wt.% Ga-doped has more basic sites, that can produce sufficient oxygen species to eliminate the coke in the reaction and show highly stability. Ni based catalyst performs high activity in methane dry reforming reaction but suffers from severe carbon deposition and deactivation. A series of CeO 2 supported Ni catalysts promoted with various amounts of Ga were synthesized, and regulated the basic site of the catalysts. The Ni/CeO 2 catalyst with 3 wt% Ga-doped shows the highest activity ( X CH 4 = 74% and X CO 2 = 88%) and stability with the H 2 /CO ratio of 0.94 after a 35-h reaction without any carbon deposition. The CH 4 -CO 2 -CH 4 pulse experiments indicate that the doping of Ga can produce enough oxygen species to eliminate the carbon deposition and maintain the catalytic activity. Superior activity with the better stability can be attributed to the enhanced CO 2 adsorption and activation over the basic site of the catalyst, which is regulated by the introduction of Ga. These results provide a fundamental understanding of the relationship between the basic site regulated by Ga and the catalyst stability the Ni/CeO 2 catalytic system. The doping of Ga successfully regulated the basicity of the Ni/CeO 2 catalyst, promoted the adsorption and activation of CO 2 , which improved the catalytic activity and stability.
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