Rational design of catalysts with earth‐abundant elements

Abstract

Catalysis has played a crucial role in energy sustainability, environment control, and chemical production, while the design of high-performance catalysts is a key scientific question. In nature, biological organisms carry out catalysis with earth-abundant metals, whereas modern industrial processes rely heavily on precious metals. This points out the necessity of designing state-ofthe-art catalysts with earth-abundant elements to maintain sustainable catalysis. In this review, we will start with the fact that nature uses earth-abundant metals to feed the planet, followed by a few successful examples of catalyst design for water oxidation. Then, we will systematically introduce the practical methods in computational catalyst design and their applications in the rational modification of EAM catalysts for various reactions. In addition, the roles of high-throughput computations and artificial intelligence in this framework are summarized and discussed. We will also discuss the potential limitations of the framework and the strategies to overcome these challenges. Finally, we emphasize the importance of the synergistic efforts between theory and experiments in rational catalyst design with earth-abundant elements.

Demagnetizing Ferromagnetic Catalysts to the Sabatier Optimal of Haber–Bosch Process

“…However, it is quite challenging to separate the electronic and geometric structure of a chemical system . Thus, these modifications can lead to reconstructions of the active center and ultimately establish a different reactivity trend for the newly designed structures. ,, Strictly speaking, none of the classical Sabatier volcanos have been truly approached underneath chemical and materials engineering, whereas it is more adequate to be described as a new Sabatier volcano. As a result, the regularities summarized from classical trends are insufficient to predict the performance of novel materials.…”

“…In heterogeneous catalysis, the Sabatier principle demonstrates that optimal catalysts have suitable binding strengths with reaction intermediates. Moreover, a volcano-like correlation can be established between catalytic performance and E ads . − Since the binding strength of adsorbates ( E ads ) is highly related to the electronic structures (e.g., the density of states of d-electrons) of the solid catalysts, , effective design strategies as alloying, strain, defect engineering, and confinement , are performed to tuning this essential quantity. However, it is quite challenging to separate the electronic and geometric structure of a chemical system .…”

The theoretical design of manganese catalysts with a Si–N–Si–C–Si–C six-membered ring core-based bowl-shaped quadridentate ligand for the hydrogenation of CO/CN bonds

“…With the development of computational chemistry methods, software including machine learning and computer hardware, computer-aided molecular design could facilitate the speed of ligand design. 29–36 In 2022, our group designed a series of Mn catalysts with quadridentate framework ligands step by step, and studied the reaction mechanisms of the AKH using the DFT method, with potential good stereoselectivity and high catalytic activity. 37…”

“…With the development of computational chemistry methods, software including machine learning and computer hardware, computer-aided molecular design could facilitate the speed of ligand design. [29][30][31][32][33][34][35][36] In 2022, our group designed a series of Mn catalysts with quadridentate framework ligands step by step, and studied the reaction mechanisms of the AKH using the DFT method, with potential good stereoselectivity and high catalytic activity. 37 In this work, a series of new bowl-shaped quadridentate framework ligands (LYG ligands) owning a Si-N-Si-C-Si-C six-membered ring core were designed (P(R 1 ) 2 CH 2 Si(CH 2 )(CH 3 )NSi(CH 3 ) (CH 2 Si(CH 3 )CH 2 P(R 3 ) 2 )CH 2 P(R 2 ) 2 ), R 1 , R 2 , R 3 = H, Me, Ph, etc.)…”

Demagnetizing Ferromagnetic Catalysts to the Sabatier Op-timal of Haber-Bosch Process

“…Moreover, a volcano-like correlation can be established between catalytic performance and Eads. [1][2][3][4] Since the binding strength of adsorbates (Eads) with solid catalysts is highly related to their electronic structures, e.g., the density of states (DOS) of d-electrons, 5,6 effective design strategies as alloying, 7 strain, 8 defect engineering, 9 and confinement 10,11 are performed to tuning this essential quantity. However, it is quite challenging to separate the electronic and geometric structure of a chemical system.…”