4.5 Article

Theoretical investigation of d-orbitals involvement in catalytic activity by incorporation of bimetallic on adjacent position

Related references

Note: Only part of the references are listed.
Article Chemistry, Multidisciplinary

Tailoring the d-Orbital Splitting Manner of Single Atomic Sites for Enhanced Oxygen Reduction

Yunkun Dai et al.

Summary: A strategy of Fe d-orbital splitting modulation by constructing axial coordination on Fe-N-4 sites is presented to regulate the electronic states of single atomic sites around the Fermi level. The axial tractions induce the distortion of Fe-N-4 SP and up to the quasi-octahedral coordination (Fe-N4O1 OCquasi), leading to electron rearrangement and diluted spin polarization. This work provides a novel understanding for improving electrocatalytic performance through orbital-scale manipulation.

ADVANCED MATERIALS (2023)

Review Chemistry, Multidisciplinary

Optimizing the Electrocatalytic Selectivity of Carbon Dioxide Reduction Reaction by Regulating the Electronic Structure of Single-Atom M-N-C Materials

Tianmi Tang et al.

Summary: Electrochemical carbon dioxide reduction reaction (CO2RR) is an efficient strategy to convert excess CO2 to value-added products. Atomically dispersed metal-nitrogen-doped carbon (M-N-C) materials are superior catalysts for CO2RR due to their unique structures. However, CO2RR is challenging due to the high energy barrier involved.

ADVANCED FUNCTIONAL MATERIALS (2022)

Article Chemistry, Physical

Toward Rational Design of Dual-Metal-Site Catalysts: Catalytic Descriptor Exploration

Chuanyi Jia et al.

Summary: Dual-metal-site catalysts (DMSCs) have great potential in heterogeneous catalysis, but the underlying relationships connecting their dual-site synergistic effects on catalytic performance remain unclear. This comprehensive first-principles study reveals that the N-3-coordinated-adjacent dual-metal model exhibits stronger synergistic and dynamic effects, leading to higher catalytic activity. Fe-containing combinations are generally more active, with Fe-Ni combination identified as the most promising candidate for CO oxidation. Electronic/spectral descriptors related to charge transfer, average charge on metals, average d-orbital center on metals, and stretching vibrational frequency of reactants are found to reflect the binding ability/stability of O-2 as lone reactant. The transferability of these descriptors to multimolecular catalysis is confirmed, providing potential design strategies for high-efficiency DMSCs.

ACS CATALYSIS (2022)

Article Materials Science, Multidisciplinary

Tailoring the d-band center of N-doped carbon nanotube arrays with Co4N nanoparticles and single-atom Co for a superior hydrogen evolution reaction

Bo Cao et al.

Summary: A 3D self-supported integrated electrode with Co4N nanoparticles and single-atom Co exhibits robust performance for the hydrogen evolution reaction due to its abundance of active sites and synergistic effects among components, optimizing the d-band center for efficient electrocatalysis.

NPG ASIA MATERIALS (2021)

Article Chemistry, Multidisciplinary

Pt Single Atoms Supported on N-Doped Mesoporous Hollow Carbon Spheres with Enhanced Electrocatalytic H2-Evolution Activity

Panyong Kuang et al.

Summary: This study demonstrates the tailoring of the electronic structure of Pt single atoms supported on N-doped mesoporous hollow carbon spheres through strong EMSI engineering, leading to the Pt-1/NMHCS composite exhibiting higher activity and stability in catalyzing the electrocatalytic hydrogen evolution reaction compared to Pt-NP and commercial Pt/C. The strong EMSI effect in a unique N-1-Pt-1-C-2 coordination structure significantly modifies the electronic structure of Pt 5d states, enhancing the reduction of adsorbed proton and facilitating H-H coupling for Pt-like HER activity.

ADVANCED MATERIALS (2021)

Article Chemistry, Physical

Tailoring the 3d-orbital electron filling degree of metal center to boost alkaline hydrogen evolution electrocatalysis

Yana Men et al.

Summary: Tailoring the 3d-orbital electron filling degree of Co center in CoP can enhance the alkaline hydrogen evolution reaction (HER) performance at the atomic level, with water dissociation step identified as the root of sluggish alkaline HER kinetics. By doping Se into CoP, remarkable HER performance was achieved, and this design principle can also be applied to other anions-doped CoP for rational design of transition metal-based electrocatalysts towards alkaline HER.

APPLIED CATALYSIS B-ENVIRONMENTAL (2021)

Article Multidisciplinary Sciences

Regulating Fe-spin state by atomically dispersed Mn-N in Fe-N-C catalysts with high oxygen reduction activity

Gege Yang et al.

Summary: The research uncovered the mechanism of the oxygen reduction reaction on dual-metal atomically dispersed Fe,Mn/N-C catalyst, demonstrating its excellent performance and durability in fuel cells and metal-air batteries.

NATURE COMMUNICATIONS (2021)

Article Chemistry, Physical

Heterogeneous Two-Atom Single-Cluster Catalysts for the Nitrogen Electroreduction Reaction

Jun-Chi Chen et al.

Summary: The electrocatalytic dinitrogen reduction reaction (NRR) has the potential to produce ammonia using renewable energies, and finding stable and efficient catalysts is crucial. Recent studies have shown that heterogeneous single-cluster catalysts (SCCs) with atomically precise active sites exhibit promising catalytic activity for NRR, and density functional theory has been used to investigate the mechanism. The study reveals the importance of factors such as the reducibility of the catalyst and the orbital interaction in N-2 absorption.

JOURNAL OF PHYSICAL CHEMISTRY C (2021)

Article Multidisciplinary Sciences

Origin of enhanced water oxidation activity in an iridium single atom anchored on NiFe oxyhydroxide catalyst

Xueli Zheng et al.

PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA (2021)

Article Chemistry, Applied

In situ surface-confined fabrication of single atomic Fe-N4 on N-doped carbon nanoleaves for oxygen reduction reaction

Xiaojing Jiang et al.

Summary: This study demonstrated a controllable in situ surface-confined strategy for the synthesis of single-atom Fe-N-4 on N-doped carbon nanoleaves, leading to high surface area and graphitization degree of L-FeNC. The abundant Fe-N-4 active sites in L-FeNC resulted in enhanced mass and charge transfer, achieving a half-wave potential of 0.89 V for oxygen reduction reaction (ORR) in 0.1 M KOH.

JOURNAL OF ENERGY CHEMISTRY (2021)

Article Chemistry, Physical

Understanding the role of axial O in CO2 electroreduction on NiN4 single-atom catalysts via simulations in realistic electrochemical environment

Xu Hu et al.

Summary: This study investigates the influence of an axial oxygen atom on graphene-supported NiN4 moiety catalysts for CO2 reduction reaction. The axial oxygen significantly promotes CO2 activation in a realistic electrochemical environment, providing a new perspective for CO2RR catalyzed by single-atom catalysts.

JOURNAL OF MATERIALS CHEMISTRY A (2021)

Article Chemistry, Multidisciplinary

Amination strategy to boost the CO2 electroreduction current density of M-N/C single-atom catalysts to the industrial application level

Zhipeng Chen et al.

Summary: Despite the high Faraday efficiency for CO production, single-atom catalysts immobilized on nitrogen-doped carbon supports demonstrate low reaction current density. A novel amination strategy significantly increases the current density for CO production, particularly the aminated Ni single-atom catalyst achieving a remarkable CO partial current density of 450 mA cm(-2) with high FE. DFT calculations and experimental research reveal that the enhanced activity is due to the regulation of electronic structure of the aminated catalysts, offering a promising method for improving current density in industrial-level single-atom catalysts for CO2RR.

ENERGY & ENVIRONMENTAL SCIENCE (2021)

Article Materials Science, Multidisciplinary

Non-noble metal single-atom catalysts with phosphotungstic acid (PTA) support: A theoretical study of ethylene epoxidation

Shamraiz Hussain Talib et al.

SCIENCE CHINA-MATERIALS (2020)

Article Chemistry, Physical

The effect of coordination environment on the kinetic and thermodynamic stability of single-atom iron catalysts

Weijie Yang et al.

PHYSICAL CHEMISTRY CHEMICAL PHYSICS (2020)

Article Chemistry, Multidisciplinary

Building Up a Picture of the Electrocatalytic Nitrogen Reduction Activity of Transition Metal Single-Atom Catalysts

Xin Liu et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2019)

Article Chemistry, Multidisciplinary

Self-Adjusting Activity Induced by Intrinsic Reaction Intermediate in Fe-N-C Single-Atom Catalysts

Yu Wang et al.

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY (2019)

Article Chemistry, Physical

Single-atom catalysts templated by metal-organic frameworks for electrochemical nitrogen reduction

Rui Zhang et al.

JOURNAL OF MATERIALS CHEMISTRY A (2019)

Article Chemistry, Multidisciplinary

Tailoring the d-Band Centers Enables Co4N Nanosheets To Be Highly Active for Hydrogen Evolution Catalysis

Zhiyan Chen et al.

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2018)

Review Multidisciplinary Sciences

Combining theory and experiment in electrocatalysis: Insights into materials design

Zhi Wei Seh et al.

SCIENCE (2017)

Article Chemistry, Multidisciplinary

Transition Metal d-Orbital Splitting Diagrams: An Updated Educational Resource for Square Planar Transition Metal Complexes

Jonas Boergel et al.

JOURNAL OF CHEMICAL EDUCATION (2016)

Article Nanoscience & Nanotechnology

Sulfur-Doped Fe/N/C Nanosheets as Highly Efficient Electrocatalysts for Oxygen Reduction Reaction

Kui Hu et al.

ACS APPLIED MATERIALS & INTERFACES (2016)

Review Chemistry, Physical

Graphene-based materials for catalysis

Bruno F. Machado et al.

CATALYSIS SCIENCE & TECHNOLOGY (2012)

Article Chemistry, Physical

Fabrication of gold nanoparticle/graphene oxide nanocomposites and their excellent catalytic performance

Nana Zhang et al.

JOURNAL OF MATERIALS CHEMISTRY (2011)

Article Chemistry, Physical

Improved Stability and Catalytic Properties of Au16 Cluster Supported on Graphane

G. Chen et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2011)

Article Materials Science, Multidisciplinary

Gold nanoparticles-graphene hybrids as active catalysts for Suzuki reaction

Yang Li et al.

MATERIALS RESEARCH BULLETIN (2010)

Article Chemistry, Physical

Metal-Embedded Graphene: A Possible Catalyst with High Activity

Yun-Hao Lu et al.

JOURNAL OF PHYSICAL CHEMISTRY C (2009)

Article Chemistry, Physical

The rise of graphene

A. K. Geim et al.

NATURE MATERIALS (2007)

Article Multidisciplinary Sciences

Electric field effect in atomically thin carbon films

KS Novoselov et al.

SCIENCE (2004)