在高透合金催化剂上解脱CO2的减少反应中间体:一种可解释的机器学习方法来建立缩放关系
Diptendu Roy1, Shyama Charan Mandal1,2,3, Amitabha Das1
1Department of Chemistry, Indian Institute of Technology Indore, Indore, 453552, India.
Chemistry (Weinheim an der Bergstrasse, Germany)
|November 15, 2023
概括
本研究引入了一种可解释的机器学习 (ML) 方法,用于预测高合金 (HEA) 表面上二氧化碳减排反应 (CO2 RR) 中间体的缩放关系,从而改进催化剂设计.
科学领域:
- 催化剂是一种催化剂.
- 材料科学 材料科学 材料科学
- 计算化学计算化学
背景情况:
- 在复杂表面,如高合金 (HEAs) 上建立反应中间体的缩放关系至关重要,但具有挑战性.
- 目前在催化中的机器学习 (ML) 模型往往缺乏可解释性,阻碍了机械理解和理性设计.
研究的目的:
- 开发一种可解释的ML方法,用于在HEA表面上建立二氧化碳还原反应 (CO2 RR) 中间体之间的缩放关系.
- 增强对复杂材料系统上的催化过程的理解和可预测性.
主要方法:
- 设计了一个可解释的ML框架,使用本地可解释的模型不可知解释 (LIME),累积的本地效应 (ALE) 和转换特征重要性 (PFI).
- 在基于CuCoNiZnMg和CuCoNiZnSn的HEA数据上反复应用和验证了ML方法.
- 采用黑子模型来解释全球和本地吸附能量.
主要成果:
- 通过使用高精度的HCO训练数据 (MAE:分别为0.24 eV和0.23 eV) 成功预测了*H2CO和*H3CO中间体的吸附能量.
- 从*H训练数据 (MAE:0.32 eV) 中准确预测了*O中间体的吸附能量.
- 在复杂的HEA表面上证明了可解释ML方法的有效性.
结论:
- 提出的可解释的ML方法成功地建立了HEAs上的CO2 RR中间体的缩放关系.
- 这种方法提供了一种途径,可以将ML的范式转变为催化,以提高可解释性和预测能力.
- 这些发现为更合理地设计二氧化碳转化催化剂铺平了道路.
相关概念视频
02:17Reduction of Alkenes: Asymmetric Catalytic Hydrogenation
3.3K
Catalytic hydrogenation of alkenes is a transition-metal catalyzed reduction of the double bond using molecular hydrogen to give alkanes. The mode of hydrogen addition follows syn stereochemistry.
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
The metal catalyst used can be either heterogeneous or homogeneous. When hydrogenation of an alkene generates a chiral center, a pair of enantiomeric products is expected to form. However, an enantiomeric excess of one of the products can be facilitated using an enantioselective reaction or an...
3.3K
02:24Reduction of Alkynes to cis-Alkenes: Catalytic Hydrogenation
7.7K
Introduction
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
Like alkenes, alkynes can be reduced to alkanes in the presence of transition metal catalysts such as Pt, Pd, or Ni. The reaction involves two sequential syn additions of hydrogen via a cis-alkene intermediate.
7.7K
02:13Reduction of Alkenes: Catalytic Hydrogenation
12.1K
Alkenes undergo reduction by the addition of molecular hydrogen to give alkanes. Because the process generally occurs in the presence of a transition-metal catalyst, the reaction is called catalytic hydrogenation.
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
Metals like palladium, platinum, and nickel are commonly used in their solid forms — fine powder on an inert surface. As these catalysts remain insoluble in the reaction mixture, they are referred to as heterogeneous catalysts.
The hydrogenation process takes place on the...
12.1K
01:20Amides to Amines: LiAlH4 Reduction
4.8K
Amide reduction with strong reducing agents like lithium aluminum hydride proceeds through a nucleophilic acyl substitution to form amines. Primary, secondary, and tertiary amides yield primary, secondary, and tertiary amines, respectively.
Amide reduction requires two equivalents of the reducing agent, acting as a source of hydride ions. As shown in the figure, the reaction is initiated with a nucleophilic attack by the hydride ion at the carbonyl carbon to form a tetrahedral intermediate.
Amide reduction requires two equivalents of the reducing agent, acting as a source of hydride ions. As shown in the figure, the reaction is initiated with a nucleophilic attack by the hydride ion at the carbonyl carbon to form a tetrahedral intermediate.
4.8K
01:22Alkenes via Reductive Coupling of Aldehydes or Ketones: McMurry Reaction
1.9K
The radical dimerization of ketones or aldehydes gives vicinal diols through a pinacol coupling reaction. However, the behavior of titanium metals used for the reaction as a source of electrons is unusual. When the reaction is carried out in the presence of titanium, diols can be isolated at low temperatures. Else titanium further reacts with diols, forming alkenes through the McMurry reaction.
1.9K
01:18Preparation of Aldehydes and Ketones from Carboxylic Acid Derivatives
2.6K
Aldehydes are more reactive than carboxylic acids and hence, can get over-reduced to alcohol in the presence of strong reducing agents. Therefore, carboxylic acids are inefficient in preparing aldehydes using LAH.
Carboxylic acid derivatives like acid chlorides and esters are more easily reducible than the corresponding acids. The derivatives reduce in the presence of mild reducing agents to give aldehydes. Aldehydes can also be prepared by Rosenmund reduction, that is, the reduction of...
Carboxylic acid derivatives like acid chlorides and esters are more easily reducible than the corresponding acids. The derivatives reduce in the presence of mild reducing agents to give aldehydes. Aldehydes can also be prepared by Rosenmund reduction, that is, the reduction of...
2.6K