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).

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.

Facile synthesis of impurity-free iron single atom catalysts for highly efficient oxygen reduction reaction and active-site identification

2019 ◽  
Vol 9 (23) ◽  
pp. 6556-6560 ◽  
Author(s):  
Qian He ◽  
Yuying Meng ◽  
Hao Zhang ◽  
Ying Zhang ◽  
Hongyu Chen ◽  
...  
Keyword(s):  
Oxygen Reduction Reaction ◽  
Oxygen Reduction ◽  
Active Site ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
Facile Synthesis ◽  
Free Iron ◽  
Highly Efficient ◽  
Site Identification

A precursor-dilution strategy is developed to prepare an impurity-free Fe single atom catalyst with superior oxygen reduction reaction catalytic performance.

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.

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 Mo-doped boron nitride monolayer as a promising single-atom electrocatalyst for CO2 conversion

2019 ◽  
Vol 10 ◽  
pp. 540-548 ◽  
Author(s):  
Qianyi Cui ◽  
Gangqiang Qin ◽  
Weihua Wang ◽  
Lixiang Sun ◽  
Aijun Du ◽  
...  
Keyword(s):  
Boron Nitride ◽  
Density Functional ◽  
Experimental Studies ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
Ambient Conditions ◽  
Functional Theory ◽  
Earth Abundant ◽  
Insight Into

The design of new, efficient catalysts for the conversion of CO2 to useful fuels under mild conditions is urgent in order to reduce greenhouse gas emissions and alleviate the energy crisis. In this work, a series of transition metals (TMs), including Sc to Zn, Mo, Ru, Rh, Pd and Ag, supported on a boron nitride (BN) monolayer with boron vacancies, were investigated as electrocatalysts for the CO2 reduction reaction (CRR) using comprehensive density functional theory (DFT) calculations. The results demonstrate that a single-Mo-atom-doped boron nitride (Mo-doped BN) monolayer possesses excellent performance for converting CO2 to CH4 with a relatively low limiting potential of −0.45 V, which is lower than most catalysts for the selective production of CH4 as found in both theoretical and experimental studies. In addition, the formation of OCHO on the Mo-doped BN monolayer in the early hydrogenation steps is found to be spontaneous, which is distinct from the conventional catalysts. Mo, as a non-noble element, presents excellent catalytic performance with coordination to the BN monolayer, and is thus a promising transition metal for catalyzing CRR. This work not only provides insight into the mechanism of CRR on the single-atom catalyst (Mo-doped BN monolayer) at the atomic level, but also offers guidance in the search for appropriate earth-abundant TMs as electrochemical catalysts for the efficient conversion of CO2 to useful fuels under ambient conditions.

scholarly journals Controllable CO2 electrocatalytic reduction via ferroelectric switching on single atom anchored In2Se3 monolayer

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Lin Ju ◽  
Xin Tan ◽  
Xin Mao ◽  
Yuantong Gu ◽  
Sean Smith ◽  
...  
Keyword(s):  
First Principles ◽  
Catalytic Performance ◽  
Reduction Reaction ◽  
Single Atom ◽  
Effective Control ◽  
First Principles Calculations ◽  
Electrocatalytic Reduction ◽  
Metal Atoms ◽  
Transition Metal Atoms ◽  
Ferroelectric Switching

AbstractEfficient and selective CO2 electroreduction into chemical fuels promises to alleviate environmental pollution and energy crisis, but it relies on catalysts with controllable product selectivity and reaction path. Here, by means of first-principles calculations, we identify six ferroelectric catalysts comprising transition-metal atoms anchored on In2Se3 monolayer, whose catalytic performance can be controlled by ferroelectric switching based on adjusted d-band center and occupation of supported metal atoms. The polarization dependent activation allows effective control of the limiting potential of CO2 reduction on TM@In2Se3 (TM = Ni, Pd, Rh, Nb, and Re) as well as the reaction paths and final products on Nb@In2Se3 and Re@In2Se3. Interestingly, the ferroelectric switching can even reactivate the stuck catalytic CO2 reduction on Zr@In2Se3. The fairly low limiting potential and the unique ferroelectric controllable CO2 catalytic performance on atomically dispersed transition-metals on In2Se3 clearly distinguish them from traditional single atom catalysts, and open an avenue toward improving catalytic activity and selectivity for efficient and controllable electrochemical CO2 reduction reaction.

scholarly journals Fabricating high-loading Fe-N4 single-atom catalysts for oxygen reduction reaction by carbon-assisted pyrolysis of metal complexes

2021 ◽  
Vol 42 (5) ◽  
pp. 753-761
Author(s):  
Jun-Sheng Jiang ◽  
He-Lei Wei ◽  
Ai-Dong Tan ◽  
Rui Si ◽  
Wei-De Zhang ◽  
...  
Keyword(s):  
Oxygen Reduction Reaction ◽  
Metal Complexes ◽  
Oxygen Reduction ◽  
Reduction Reaction ◽  
High Loading ◽  
Single Atom

scholarly journals Regulating coordination number in atomically dispersed Pt species on defect-rich graphene for n-butane dehydrogenation reaction

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Xiaowen Chen ◽  
Mi Peng ◽  
Xiangbin Cai ◽  
Yunlei Chen ◽  
Zhimin Jia ◽  
...  
Keyword(s):  
Coordination Number ◽  
Density Functional ◽  
Activation Barrier ◽  
Density Functional Theory Calculation ◽  
Catalytic Performance ◽  
Atomic Level ◽  
Metal Nanoparticle ◽  
Single Atom ◽  
Nano Structure ◽  
Theory Calculation

AbstractMetal nanoparticle (NP), cluster and isolated metal atom (or single atom, SA) exhibit different catalytic performance in heterogeneous catalysis originating from their distinct nanostructures. To maximize atom efficiency and boost activity for catalysis, the construction of structure–performance relationship provides an effective way at the atomic level. Here, we successfully fabricate fully exposed Pt3 clusters on the defective nanodiamond@graphene (ND@G) by the assistance of atomically dispersed Sn promoters, and correlated the n-butane direct dehydrogenation (DDH) activity with the average coordination number (CN) of Pt-Pt bond in Pt NP, Pt3 cluster and Pt SA for fundamentally understanding structure (especially the sub-nano structure) effects on n-butane DDH reaction at the atomic level. The as-prepared fully exposed Pt3 cluster catalyst shows higher conversion (35.4%) and remarkable alkene selectivity (99.0%) for n-butane direct DDH reaction at 450 °C, compared to typical Pt NP and Pt SA catalysts supported on ND@G. Density functional theory calculation (DFT) reveal that the fully exposed Pt3 clusters possess favorable dehydrogenation activation barrier of n-butane and reasonable desorption barrier of butene in the DDH reaction.

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