中南大学林璋团队报道了一个被忽视的天然析氢途径,即低温蛇纹石化过程中Ni2+促进Fe(OH)2氧化还原H2O。相关研究成果于2021年9月14日发表在《德国应用化学》。
天然氢(H2)作为一种可再生能源,在缓解全球日益增长的环境问题方面受到了广泛关注。低温蛇纹石化(<200℃)是一种典型的水岩反应,是天然氢的主要来源。然而,天然H2的反应机理和控制步骤尚不清楚,阻碍了天然H2的进一步利用。
该文中,研究人员证明了在低温蛇纹石化过程中,可以通过Fe(OH)2氧化来确定H2的生成速率。此外,Ni2+的共存可以大大提高H2的生成动力学。当仅添加1%的Ni2+时,在90°C下,H2生成率显著提高约两个数量级。D2O同位素实验和理论计算表明,提高的H2生成动力学可归因于Ni2+促进H2O还原的催化作用。
附:英文原文
Title: An Overlooked Natural Hydrogen Evolution Pathway: Ni2+ Boosting H2O Reduction by Fe(OH)2 Oxidation during Low-temperature Serpentinization
Author: Han Song, Xinwen Ou, Bin Han, Haoyu Deng, Wenchao Zhang, Chen Tian, Chunfang Cai, Anhuai Lu, Zhang Lin, Liyuan Chai
Issue&Volume: 2021-09-14
Abstract: Natural hydrogen (H 2 ) has gained considerable attentions as a renewable energy resource to mitigate the globally increasing environmental concerns. Low-temperature serpentinization (< 200 ° C) as a typical water-rock reaction is a major source of the natural H 2 . However, the reaction mechanism and the controlling step to product H 2 remained unclear, which hinders the further utilization of natural H 2 . Herein, we demonstrated that the H 2 production rate could be determined by the Fe(OH) 2 oxidation during low-temperature serpentinization. Moreover, the co-existence of Ni 2+ could largely enhance the H 2 production kinetics. With the addition of only 1 % Ni 2+ , the H 2 production rate was remarkably enhanced by about two orders of magnitude at 90 ° C. D 2 O isotopic experiment and theoretical calculations revealed that the enhanced H 2 production kinetics could be attributed to the catalytic role of Ni 2+ to promote the reduction of H 2 O.
DOI: 10.1002/anie.202110653
Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202110653