Dandan Yang , Fan Xu , Daoming Jin , Xin Meng , Ailun Lv , Wenhua Dai , Rui Zhao , Zhong Xin
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引用次数: 0
Abstract
Developing a stable and effective Ni-based catalyst for low-temperature CO2 methanation remains a significant challenge. This study presents the synthesis of a range of MgO-promoted Ni-based catalysts supported on natural halloysite nanotubes (HNTs) through a sol-gel method assisted by citric acid. At 275°C, Ni-Mg/HNTs-1.0 CA exhibits the highest CO2 conversion (88.5%) and CH4 selectivity (98.4%). The sufficient basic sites and Ni0 sites of Ni-Mg/HNTs-1.0CA are beneficial for CO2 activation and H2 dissociation, leading to high activity at low temperatures. Additionally, Ni-Mg/HNTs-1.0 CA exhibits better anti-sintering ability during 100 h reaction, attributed to the increased interaction between metal and support. The in-situ DRIFTS results show that Ni-Mg/HNTs-1.0 CA mainly follows both formate and CO pathways, and the rapid transformation of intermediates causes superior catalytic performance. This work offers a rational design of stable and active catalysts for low-temperature CO2 methanation.
为低温二氧化碳甲烷化开发稳定有效的镍基催化剂仍然是一项重大挑战。本研究通过柠檬酸辅助溶胶-凝胶法,合成了一系列以天然海泡石纳米管(HNTs)为支撑的氧化镁促进镍基催化剂。275°C 时,Ni-Mg/HNTs-1.0 CA 的二氧化碳转化率(88.5%)和甲烷选择性(98.4%)最高。Ni-Mg/HNTs-1.0 CA 具有充足的碱性位点和 Ni0 位点,有利于 CO2 活化和 H2 解离,从而在低温下具有高活性。此外,Ni-Mg/HNTs-1.0 CA 在 100 小时的反应过程中表现出更好的抗烧结能力,这归因于金属与支撑物之间相互作用的增强。原位 DRIFTS 结果表明,Ni-Mg/HNTs-1.0 CA 主要遵循甲酸酯和 CO 两种途径,中间产物的快速转化使其具有优异的催化性能。这项工作为低温 CO2 甲烷化提供了稳定、活性催化剂的合理设计。
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods