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Boosting the direct conversion of NH4HCO3 electrolyte to syngas on Ag/Zn zeolitic imidazolate framework derived nitrogen-carbon skeleton
Frontiers of Chemical Science and Engineering ( IF 4.3 ) Pub Date : 2023-04-26 , DOI: 10.1007/s11705-022-2289-1
Huiyi Li , Jianmin Gao , Jingjing Shan , Qian Du , Yu Zhang , Xin Guo , Shaohua Wu , Zhijiang Wang

The electrochemical reduction of NH4HCO3 to syngas can bypass the high energy consumption of high-purity CO2 release and compression after the ammonia-based CO2 capture process. This technology has broad prospects in industrial applications and carbon neutrality. A zeolitic imidazolate framework-8 precursor was introduced with different Ag contents via colloid chemical synthesis. This material was carbonized at 1000 °C to obtain AgZn zeolitic imidazolate framework derived nitrogen carbon catalysts, which were used for the first time for boosting the direct conversion of NH4HCO3 electrolyte to syngas. The AgZn zeolitic imidazolate framework derived nitrogen carbon catalyst with a Ag/Zn ratio of 0.5:1 achieved the highest CO Faradaic efficiency of 52.0% with a current density of 1.15 mA·cm−2 at −0.5 V, a H2/CO ratio of 1–2 (−0.5 to −0.7 V), and a stable catalytic activity of more than 6 h. Its activity is comparable to that of the CO2-saturated NH4HCO3 electrolyte. The highly discrete Ag-Nx and Zn-Nx nodes may have combined catalytic effects in the catalysts synthesized by appropriate Ag doping and sufficient carbonization. These nodes could increase active sites of catalysts, which is conducive to the transport and adsorption of reactant CO2 and the stability of *COOH intermediate, thus can improve the selectivity and catalytic activity of CO.



中文翻译:

在 Ag/Zn 沸石咪唑酯骨架衍生的氮碳骨架上促进 NH4HCO3 电解液直接转化为合成气

NH 4 HCO 3电化学还原为合成气可以绕过基于氨的CO 2捕获过程后高纯度CO 2释放和压缩的高能耗。该技术在工业应用和碳中和方面具有广阔的前景。通过胶体化学合成引入具有不同银含量的沸石咪唑酯骨架-8 前体。将该材料在1000℃下碳化得到AgZn沸石咪唑骨架衍生的氮碳催化剂,首次用于促进NH 4 HCO 3直接转化电解质合成气。Ag/Zn 比为 0.5:1 的 AgZn 沸石咪唑盐骨架衍生氮碳催化剂在 -0.5 V、H 2 /CO 比下以 1.15 mA·cm -2 的电流密度实现了 52.0% 的最高CO法拉第效率1-2(-0.5 至-0.7 V),以及超过 6 小时的稳定催化活性。其活性与CO 2饱和的NH 4 HCO 3电解质的活性相当。高度离散的 Ag-N x和 Zn-N x节点可能在通过适当的 Ag 掺杂和充分的碳化合成的催化剂中具有联合催化作用。这些节点可以增加催化剂的活性位点,有利于反应物CO 2的输送和吸附以及*COOH中间体的稳定性,从而提高CO的选择性和催化活性。

更新日期:2023-04-27
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