首页|HCl在Au(111)表面覆盖量相关的解离吸附研究

HCl在Au(111)表面覆盖量相关的解离吸附研究

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HCl在Au(111)表面的解离吸附己成为表面化学研究中的一个未解之谜.尽管过去几年中科学家们进行了大量努力,但各种理论模型仍然严重高估了零覆盖下初始吸附概率.为了找出实验与理论之间巨大差异的根源,本文利用新设计的分子束-表面装置并结合理论计算重新开展了HCl在 Au(111)上的解离吸附研究.通过改变HCl的入射剂量进行Cl覆盖量测量所得的零覆盖解离系数与先前的实验结果相符.然而,在低覆盖量范围内,随着HCl剂量的增加,覆盖量/剂量斜率出现了急剧变化,这可能会导致对拟合的零覆盖初始吸附概率数值产生一些不确定性,这似乎与密度泛函理论在低Cl覆盖量下预测的解离势垒的覆盖量依赖性一致.本文结果揭示了利用有限覆盖的模拟与该系统中零覆盖的实验数据进行比较的潜在不一致性,提供了改进实验和理论的思路.
Coverage Dependent Dissociative Adsorption of HCl on Au(111)
Dissociative adsorption of HCl on Au(111)has become one of un-solved puzzles in surface chemistry.Despite tremendous efforts in the past years,various theoretical models still greatly overestimate the zero-coverage initial sticking probabilities(S0).To find the ori-gin of the large experiment-theory discrepancy,we have revisited the dissociative adsorption of HCl on Au(111)with a newly de-signed molecular beam-surface apparatus.The zero-coverage S0 derived from Cl-coverage measurements with varying HCl doses agree well with previous ones.However,we notice a sharp change of the coverage/dose slope with the HCl dosage at the low coverage regime,which may result in some uncertainties to the fitted S0 value.This seems consistent with a coverage-dependence of the dissociation barrier predicted by density functional theory at low Cl-coverages.Our results reveal the potential inconsistency of utilizing simulations with fi-nite coverage to compare against experimental data with zero coverage in this system,and provide guidance for improving both experiment and theory in this regard.

Dissociative adsorptionReaction probabilityMolecular beamDensity func-tional theory

申琦琦、朱玲君、吴家伟、董文锐、王兴安、汪涛、蒋彬、杨学明

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中国科学院大连化学物理研究所,分子反应动力学国家重点实验室,大连 116023

中国科学院大学化学科学学院,北京 100049

中国科学技术大学精准智能化学重点实验室,合肥 230026

中国科学技术大学化学物理系,合肥 230026

合肥国家实验室,合肥 230088

南方科技大学理学院化学系,深圳 518055

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解离吸附 反应概率 分子束 密度泛函理论

National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaInnovation program for Quantum Science and TechnologyGuangdong Science and Technology ProgramGuangdong Science and Technology ProgramShenzhen Science and Technology ProgramStrategic Priority Research Program of the Chinese Academy of Sciences

221730422197303722073089223278012021ZD03033042019ZT08L4552019JC01X091ZDSYS20200421111001787XDB0450101

2024

10.1063/1674-0068/cjcp2312145

化学物理学报(英文版)
中国物理学会

化学物理学报(英文版)

CSTPCDEI
影响因子：0.162
ISSN：1674-0068
年,卷(期)：2024.37(4)