基于DFT和机器学习的单原子合金催化剂的设计与筛选

IF 3.5 3区 工程技术 Q2 ENGINEERING, CHEMICAL AIChE Journal Pub Date : 2024-12-10 DOI:10.1002/aic.18678
Wenyu Zhou, Haisong Feng, Shihong Zhou, Mengxin Wang, Yuping Chen, Chenyang Lu, Hao Yuan, Jing Yang, Qun Li, Luxi Tan, Lichun Dong, Yong-Wei Zhang
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引用次数: 0

摘要

二氧化碳(CO2)利用技术对于实现碳中和具有重要意义,其中催化材料起着至关重要的作用,其中单原子合金(SAAs)尤其受到关注。在本研究中,采用密度泛函理论(DFT)计算和机器学习来评估Cu-, Ag-和ni -宿主SAAs作为电化学CO2还原为CH3OH催化剂的有效性。本文计算了35个碳还原过程中477个基本反应的吉布斯自由能,并利用该数据集建立了训练好的梯度增强回归模型。随后,预测了46种未知的SAAs的性质,包括它们的途径、产物、势决定步骤(PDS)和相应的势决定步骤(GPDS)的吉布斯自由能(GPDS)。ZnCu、AuAg和MoNi这三种很有希望的候选材料,分别因其在Cu、Ag和Ni托管SAAs中最低的gds而脱颖而出。
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Designing and screening single-atom alloy catalysts for CO2 reduction to CH3OH via DFT and machine learning
Carbon dioxide (CO2) utilization technology is of great significance for achieving carbon neutrality, in which the catalytic materials play crucial roles, and among them, single-atom alloys (SAAs) are of particular interests. In this study, density functional theory (DFT) calculations and machine learning are employed to assess the effectiveness of Cu-, Ag-, and Ni-host SAAs as catalysts for electrochemical CO2 reduction to CH3OH. The Gibbs free energies of 477 elementary reactions across 35 SAAs involved in CO2 reduction are calculated, and by utilizing this dataset, a trained gradient boosting regression model is established with an excellent accuracy. Subsequently, the properties of 46 unknown SAAs are predicted, including their pathways, products, potential-determining steps (PDS), and corresponding Gibbs free energies of the PDS (GPDS). Three promising candidates, ZnCu, AuAg and MoNi, stand out due to their lowest GPDS among Cu-, Ag- and Ni- hosted SAAs, respectively.
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来源期刊
AIChE Journal
AIChE Journal 工程技术-工程:化工
CiteScore
7.10
自引率
10.80%
发文量
411
审稿时长
3.6 months
期刊介绍: The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.
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