Double-atom catalysts for energy-related electrocatalysis applications: a theoretical perspective

2022 ◽  
Author(s):  
Donghai Wu ◽  
Bingling He ◽  
Yuanyuan Wang ◽  
Peng Lv ◽  
Dongwei Ma ◽  
...  
Keyword(s):  
Rational Design ◽  
Synergetic Effect ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Atomic Scale ◽  
Theoretical Research ◽  
Single Atom ◽  
Research Attention ◽  
Wide Range ◽  
Electrocatalytic Reactions

Abstract Due to the excellent activity, selectivity, and stability, atomically dispersed metal catalysts with well-defined structures have attracted intensive research attention. As the extension of single-atom catalyst (SAC), double-atom catalyst (DAC) has recently emerged as a research focus. Compared with SAC, the higher metal loading, more complicated and flexible active site, easily tunable electronic structure, and the synergetic effect between two metal atoms could provide DACs with better catalytic performance for a wide range of catalytic reactions. This review aims to summarize the recent advance in theoretical research on DACs for diverse energy-related electrocatalytic reactions. It starts with a brief introduction to DACs. Then an overview of the main experimental synthesis strategies of DACs is provided. Emphatically, the catalytic performance together with the underlying mechanism of the different electrocatalytic reactions, including nitrogen reduction reaction, carbon dioxide reduction reaction, oxygen reduction reaction, and oxygen and hydrogen evolution reactions, are highlighted by discussing how the outstanding attributes mentioned above affect the reaction pathway, catalytic activity, and product selectivity. Finally, the opportunities and challenges for the development of DACs are prospected to shed fresh light on the rational design of more efficient catalysts at the atomic scale in the future.

scholarly journals Morphological Attributes Govern CO2 Reduction on Mesoporous Carbon Nanosphere with Embedded Axial Co-N5 Sites

2021 ◽  
Author(s):  
Youzhi Li ◽  
Bo Wei ◽  
Zhongjian Li ◽  
Lei Fan ◽  
Qike Jiang ◽  
...  
Keyword(s):  
Mesoporous Carbon ◽  
High Performance ◽  
Density Functional ◽  
Rational Design ◽  
Co2 Reduction ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
High Turnover ◽  
Morphological Attributes

Abstract Although single-atom catalysts (SACs) have been widely employed in the CO2 reduction reaction (CO2RR), the understanding regarding the effect of morphological attributes on catalytic performance are still lacking, which prevents the rational design of high-performance catalysts for electrochemical CO2RR. Here, we developed a novel catalyst with axial Co-N5 sites embedded on controllable mesoporous carbon nanosphere with different graded pore structures. Benefiting from the precise control of porosity, the influence of morphological attributes on catalytic performance was well revealed. In situ characterization combined with density functional theory (DFT) calculations revealed that axial N-coordination induced local d-p orbitals coupling enhancement of Co with oxides and the optimal pore size of 27 nm promoted the interfacial bonding characteristics, which facilitate both the COOH* generation and CO desorption. Consequently, A superior selectivity of nearly 100% at -0.8 V vs. RHE and commercially relevant current densities of >150 mA cm−2 could be achieved, and a strikingly high turnover frequency of 1.136*104 h−1 at -1.0 V has been obtained, superior to the most of Co-based catalysts.

A rational study on the geometric and electronic properties of single-atom catalysts for enhanced catalytic performance

Nanoscale ◽  
2020 ◽  
Vol 12 (45) ◽  
pp. 23206-23212
Author(s):  
Qi Xue ◽  
Yi Xie ◽  
Simson Wu ◽  
Tai-Sing Wu ◽  
Yun-Liang Soo ◽  
...  
Keyword(s):  
Electronic Properties ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
Geometric And Electronic Properties

We investigate the geometric and electronic properties of single-atom catalysts (SACs) for electrocatalytic CO2 reduction reaction (eCO2RR).

scholarly journals A Mini Review of the Preparation and Photocatalytic Properties of Two-Dimensional Materials

2020 ◽  
Vol 8 ◽  
Author(s):  
Shuhua Hao ◽  
Xinpei Zhao ◽  
Qiyang Cheng ◽  
Yupeng Xing ◽  
Wenxuan Ma ◽  
...  
Keyword(s):  
Active Sites ◽  
2D Materials ◽  
Chemical Properties ◽  
Metal Sulfide ◽  
Catalytic Performance ◽  
Theoretical Research ◽  
Single Atom ◽  
Preparation Methods ◽  
Two Dimensional Materials ◽  
Physical And Chemical

The successful preparation and application of graphene shows that it is feasible for the materials with a thickness of a single atom or few atomic layers to exist stably in nature. These materials can exhibit unusual physical and chemical properties due to their special dimension effects. At present, researchers have made great achievements in the preparation, characterization, modification, and theoretical research of 2D materials. Because the structure of 2D materials is often similar, it has a certain degree of qualitative versatility. Besides, 2D materials often carry good catalytic performance on account of their more active sites and adjustable harmonic electronic structure. In this review, taking 2D materials as examples [graphene, boron nitride (h-BN), transition metal sulfide and so on], we review the crystal structure and preparation methods of these materials in recent years, focus on their photocatalyst properties (carbon dioxide reduction and hydrogen production), and discuss their applications and development prospects in the future.

The synergetic effect of aqua ligand and metal site on performance of single-atom catalysts in H2O2 synthesis: a Density Functional Theory Study

2022 ◽  
Author(s):  
Xin-Chen Zhu ◽  
Wei Zhang ◽  
Qian Xia ◽  
Anfu Hu ◽  
Jian Jiang ◽  
...  
Keyword(s):  
Density Functional Theory ◽  
Density Functional ◽  
Rational Design ◽  
Synergetic Effect ◽  
Density Functional Theory Calculations ◽  
Single Atom ◽  
Density Functional Theory Study ◽  
Functional Theory ◽  
Metal Site ◽  
Coordination Field

To study the effect of coordination field on catalytic property is critical for rational design of outstanding electrocatalyst for H2O2 synthesis. Herein, via density functional theory calculations, we built an...

Rational design of three-dimensional nitrogen-doped carbon nanoleaf networks for high-performance oxygen reduction

2015 ◽  
Vol 3 (10) ◽  
pp. 5617-5627 ◽  
Author(s):  
Liang Chen ◽  
Chenyu Xu ◽  
Ran Du ◽  
Yueyuan Mao ◽  
Cheng Xue ◽  
...  
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
High Performance ◽  
Rational Design ◽  
Three Dimensional ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Nitrogen Doped ◽  
Nitrogen Doped Carbon ◽  
Excellent Catalytic Performance

“Carbon nanoleaf” aerogels were developed, constructed with nitrogen-doped CNTs/GNRs, which show excellent catalytic performance in oxygen reduction reaction.

scholarly journals Ruthenium Supported on Ionically Cross-linked Chitosan-Carrageenan Hybrid MnFe2O4 Catalysts for 4-Nitrophenol Reduction

Catalysts ◽  
2019 ◽  
Vol 9 (3) ◽  
pp. 254 ◽  
Author(s):  
Kin Hong Liew ◽  
Tian Khoon Lee ◽  
Mohd Ambar Yarmo ◽  
Kee Shyuan Loh ◽  
Andreia F. Peixoto ◽  
...  
Keyword(s):  
Catalytic Activity ◽  
Electrostatic Interactions ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Ru Nanoparticles ◽  
Nitrophenol Reduction ◽  
Active Metal ◽  
Wide Range ◽  
Mnfe2o4 Nanoparticles ◽  
Superparamagnetic Properties

Herein, we report a facile procedure to synthesize the hybrid magnetic catalyst (Ru@CS-CR@Mn) using ruthenium (Ru) supported on ionically cross-linked chitosan-carrageenan (CS-CR) and manganese ferrite (MnFe2O4) nanoparticles with excellent catalytic activity. The ionic gelation of CS-CR is acting as a protecting layer to promote the encapsulation of MnFe2O4 and Ru nanoparticles by electrostatic interactions. The presence of an active metal and a CS-CR layer on the as-prepared Ru@CS-CR@Mn catalyst was well determined by a series of physicochemical analyses. Subsequently, the catalytic performances of the Ru@CS-CR@Mn catalysts were further examined in the 4-nitrophenol (4-NP) reduction reaction in the presence of sodium borohydride (reducing agent) at ambient temperature. The Ru@CS-CR@Mn catalyst performed excellent catalytic activity in the 4-NP reduction, with a turnover frequency (TOF) values of 925 h−1 and rate constant (k) of 0.078 s−1. It is worth to mentioning that the Ru@CS-CR@Mn catalyst can be recycled and reused up to at least ten consecutive cycles in the 4-NP reduction with consistency in catalytic performance. The Ru@CS-CR@Mn catalyst is particularly attractive as a catalyst due to its superior catalytic activity and superparamagnetic properties for easy separation. We foresee this catalyst having high potential to be extended in a wide range of chemistry applications.

Coordination tunes the activity and selectivity of the nitrogen reduction reaction on single-atom iron catalysts: a computational study

2021 ◽  
Author(s):  
Dongxu Jiao ◽  
Yuejie Liu ◽  
Qinghai Cai ◽  
Jingxiang Zhao
Keyword(s):  
Computational Study ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
Iron Catalysts ◽  
Nitrogen Reduction

By introducing B coordination, the catalytic performance of Fe-N4/G can be greatly enhanced.

scholarly journals A general strategy for preparing pyrrolic-N4 type single-atom catalysts via pre-located isolated atoms

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Junjie Li ◽  
Ya-fei Jiang ◽  
Qi Wang ◽  
Cong-Qiao Xu ◽  
Duojie Wu ◽  
...  
Keyword(s):  
Active Sites ◽  
Density Functional ◽  
Rational Design ◽  
Catalytic Performance ◽  
Single Atom ◽  
General Strategy ◽  
New Findings ◽  
Synthesis Strategy ◽  
Structure Density ◽  
Application Fields

AbstractSingle-atom catalysts (SACs) have been applied in many fields due to their superior catalytic performance. Because of the unique properties of the single-atom-site, using the single atoms as catalysts to synthesize SACs is promising. In this work, we have successfully achieved Co1 SAC using Pt1 atoms as catalysts. More importantly, this synthesis strategy can be extended to achieve Fe and Ni SACs as well. X-ray absorption spectroscopy (XAS) results demonstrate that the achieved Fe, Co, and Ni SACs are in a M1-pyrrolic N4 (M= Fe, Co, and Ni) structure. Density functional theory (DFT) studies show that the Co(Cp)2 dissociation is enhanced by Pt1 atoms, thus leading to the formation of Co1 atoms instead of nanoparticles. These SACs are also evaluated under hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), and the nature of active sites under HER are unveiled by the operando XAS studies. These new findings extend the application fields of SACs to catalytic fabrication methodology, which is promising for the rational design of advanced SACs.

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