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氢化钛中的晶格氢转移增强了电催化硝酸盐向氨的转化。

Lattice hydrogen transfer in titanium hydride enhances electrocatalytic nitrate to ammonia conversion.

作者信息

Li Jiawei, Yu Wanqiang, Yuan Haifeng, Wang Yujie, Chen Yuke, Jiang Di, Wu Tong, Song Kepeng, Jiang Xuchuan, Liu Hong, Hu Riming, Huang Man, Zhou Weijia

机构信息

Institute for Advanced Interdisciplinary Research (iAIR), School of Chemistry and Chemical Engineering, University of Jinan, Jinan, P. R. China.

Electron Microscopy Center, Shandong University, Jinan, Shandong, P. R. China.

出版信息

Nat Commun. 2024 Nov 3;15(1):9499. doi: 10.1038/s41467-024-53833-x.

Abstract

The electrocatalytic reduction of nitrate toward ammonia under mild conditions addresses many challenges of the Haber-Bosch reaction, providing a sustainable method for ammonia synthesis, yet it is limited by sluggish reduction kinetics and multiple competing reactions. Here, the titanium hydride electrocatalyst is synthesized by electrochemical hydrogenation reconstruction of titanium fiber paper, which achieves a large ammonia yield rate of 83.64 mg h cm and a high Faradaic efficiency of 99.11% with an ampere-level current density of 1.05 A cm at -0.7 V versus the reversible hydrogen electrode. Electrochemical evaluation and kinetic studies indicate that the lattice hydrogen transfer from titanium hydride promotes the electrocatalytic performance of nitrate reduction reaction and the reversible equilibrium reaction between lattice hydrogen and activate hydrogen not only improves the electrocatalytic activity of nitrate reduction reaction but also demonstrates notable catalytic stability. These finding offers a universal design principle for metal hydrides as catalysts for effectively electrochemical ammonia production, highlighting their potential for sustainable ammonia synthesis.

摘要

在温和条件下将硝酸盐电催化还原为氨解决了哈伯-博施法反应的诸多挑战,为氨合成提供了一种可持续的方法,但它受到缓慢的还原动力学和多个竞争反应的限制。在此,通过钛纤维纸的电化学氢化重构合成了氢化钛电催化剂,在相对于可逆氢电极-0.7 V的条件下,以1.05 A cm的安培级电流密度实现了83.64 mg h cm的高氨产率和99.11%的高法拉第效率。电化学评估和动力学研究表明,来自氢化钛的晶格氢转移促进了硝酸盐还原反应的电催化性能,晶格氢与活化氢之间的可逆平衡反应不仅提高了硝酸盐还原反应的电催化活性,还表现出显著的催化稳定性。这些发现为金属氢化物作为有效电化学制氨催化剂提供了一种通用的设计原则,突出了它们在可持续氨合成方面的潜力。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5886/11532501/502e1c324b58/41467_2024_53833_Fig1_HTML.jpg

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