The mechanism of interactions between H2 and CH4 dissociative adsorption on the surface of pipeline steel

IF 6.3 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Applied Surface Science Pub Date : 2025-03-20 DOI:10.1016/j.apsusc.2025.162967

Yulin Song , Cailin Wang , Cuiwei Liu , Xiusai Xu , Xiusong Huang , Yuxing Li

{"title":"The mechanism of interactions between H2 and CH4 dissociative adsorption on the surface of pipeline steel","authors":"Yulin Song , Cailin Wang , Cuiwei Liu , Xiusai Xu , Xiusong Huang , Yuxing Li","doi":"10.1016/j.apsusc.2025.162967","DOIUrl":null,"url":null,"abstract":"<div><div>The utilization of repurposing natural gas pipeline steels for hydrogen transportation requires consideration of the risk of hydrogen embrittlement (HE). The occurrence of HE begins with the initial process of hydrogen dissociative adsorption. However, due to the complicated gaseous environment, the interactions between CH4 and H2 adsorption on pipeline surfaces continue to be controversial. In this study, the influence of CH4 on H2 surface adsorption was demonstrated by the in-situ hydrogen permeation test on 20# steel. Based on Electron Backscatter Diffraction results, the interactions of H2 and CH4 adsorption on Fe(100) and high-angle grain boundary (HAGB) surfaces were calculated by DFT methods. The results determine the possibility of CH4 dissociative adsorption on the pipeline surface and reveal that H2 promotes the dissociative adsorption of CH4 on HAGBs, whereas CH4 inhibits the dissociative adsorption of H2. Moreover, the inhibitory effect of CH4 on the dissociative adsorption of H2 is positively correlated with the adsorption time of CH4 on the surface. The mechanism of interactions between CH4 and H2 was clarified that CH4 increases the energy barrier of dissociative adsorption of H2. In turn, the pre-adsorbed H2 can change the charge of HAGB surface, increasing the electrons available for CH4 dissociative adsorption.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"697 ","pages":"Article 162967"},"PeriodicalIF":6.3000,"publicationDate":"2025-03-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169433225006816","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}

引用次数: 0

Abstract

The utilization of repurposing natural gas pipeline steels for hydrogen transportation requires consideration of the risk of hydrogen embrittlement (HE). The occurrence of HE begins with the initial process of hydrogen dissociative adsorption. However, due to the complicated gaseous environment, the interactions between CH₄ and H₂ adsorption on pipeline surfaces continue to be controversial. In this study, the influence of CH₄ on H₂ surface adsorption was demonstrated by the in-situ hydrogen permeation test on 20# steel. Based on Electron Backscatter Diffraction results, the interactions of H₂ and CH₄ adsorption on Fe(100) and high-angle grain boundary (HAGB) surfaces were calculated by DFT methods. The results determine the possibility of CH₄ dissociative adsorption on the pipeline surface and reveal that H₂ promotes the dissociative adsorption of CH₄ on HAGBs, whereas CH₄ inhibits the dissociative adsorption of H₂. Moreover, the inhibitory effect of CH₄ on the dissociative adsorption of H₂ is positively correlated with the adsorption time of CH₄ on the surface. The mechanism of interactions between CH₄ and H₂ was clarified that CH₄ increases the energy barrier of dissociative adsorption of H₂. In turn, the pre-adsorbed H₂ can change the charge of HAGB surface, increasing the electrons available for CH₄ dissociative adsorption.

Abstract Image

查看原文本刊更多论文

将天然气管道钢重新用于氢气运输需要考虑氢脆（HE）的风险。氢脆的发生始于最初的氢离解吸附过程。然而，由于气体环境复杂，管道表面吸附的 CH4 和 H2 之间的相互作用仍存在争议。本研究通过对 20# 钢进行原位氢渗透试验，证明了 CH4 对 H2 表面吸附的影响。基于电子反向散射衍射结果，用 DFT 方法计算了 H2 和 CH4 在 Fe(100) 和高角度晶界 (HAGB) 表面吸附的相互作用。结果确定了管道表面解离吸附 CH4 的可能性，并揭示了 H2 促进 HAGB 上 CH4 的解离吸附，而 CH4 则抑制 H2 的解离吸附。此外，CH4 对 H2 解离吸附的抑制作用与 CH4 在表面上的吸附时间呈正相关。研究阐明了 CH4 与 H2 的相互作用机理，即 CH4 增加了 H2 解离吸附的能量势垒。反过来，预吸附的 H2 可以改变 HAGB 表面的电荷，从而增加可用于离解吸附 CH4 的电子。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.