Homonuclear multi-atom catalysts for CO<sub>2</sub> electroreduction: a comparison density functional theory study with their single-atom counterparts

Xiao, Jingjing; Liu, Ziyang; Wang, Xinshuang; Li, Fengyu; Zhao, Zhonglong

doi:10.1039/d3ta05498e

Cited by 7 publications

(3 citation statements)

References 72 publications

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“…Also, a triangular Fe3-TAC on a graphdiyne substrate is reported for N 2 reduction reaction (NRR) giving rise to the theoretical onset potential of 0.37 V RHE toward NH 3 production, which can be compared with onset potentials of 1.37 V RHE for Fe2-DAC and 1.16 V RHE for Fe-SAC . A triangular Rh3-TAC on Mo 2 CO 2 MXene is reported for CO 2 RR with an onset potential of 0.15 V RHE toward CH 4 while Os3-TAC is reported to produce C 2 H 5 OH with an onset potential of 0.48 V RHE . A triangular ZnCoFe-TAC on nitrogen-doped carbon was synthesized and theoretically investigated for the ORR and OER, showing a low OER overpotential of 0.37 V RHE at 10 mA cm –2 .…”

Section: Introductionmentioning

confidence: 94%

“…49 A triangular Rh3-TAC on Mo 2 CO 2 MXene is reported for CO 2 RR with an onset potential of 0.15 V RHE toward CH 4 while Os3-TAC is reported to produce C 2 H 5 OH with an onset potential of 0.48 V RHE . 50 A triangular ZnCoFe-TAC on nitrogen-doped carbon was synthesized and theoretically investigated for the ORR and OER, showing a low OER overpotential of 0.37 V RHE at 10 mA cm −2 . 42 A triangular Fe3@PC6 was theoretically studied for CO 2 RR toward CH 4 product with the overpotential of 0.28 V. 51 In addition, a triangular Fe3-TAC was theoretically studied and experimentally synthesized for the reduction of sulfur for Li− sulfur battery application.…”

Section: ■ Introductionmentioning

confidence: 99%

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Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Tamtaji,

Kwon,

Musgrave

et al. 2024

ACS Appl. Mater. Interfaces

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The carbon monoxide reduction reaction (CORR) toward C 2+ and C 3+ products such as propylene and cyclopropane can not only reduce anthropogenic emissions of CO and CO 2 but also produce value-added organic chemicals for polymer and pharmaceutical industries. Here, we introduce the concept of triple atom catalysts (TACs) that have three intrinsically strained and active metal centers for reducing CO to C 3+ products. We applied grand canonical potential kinetics (GCP-K) to screen 12 transition metals (M) supported by nitrogen-doped graphene denoted as M3N7, where M stands for Mn, Fe, Co, Ni, Cu, Ru, Rh, Pd, Ag, Ir, Pt, and Au. We sought catalysts with favorable CO binding, hydrogen binding, and C−C dimerization energetics, identifying Fe3N7 and Ir3N7 as the best candidates. We then studied the entire reaction mechanism from CO to C 3 H 6 and C 2 H 4 as a function of applied potential via, respectively, 12-electron and 8-electron transfer pathways on Fe3N7 and Ir3N7. Density functional theory (DFT) predicts an overpotential of 0.17 V RHE for Fe3N7 toward propylene and an overpotential of 0.42 V RHE toward cyclopropane at 298.15 K and pH = 7. Also, DFT predicts an overpotential of 0.15 V RHE for Ir3N7 toward ethylene. This work provides fundamental insights into the design of advanced catalysts for C 2+ and C 3+ synthesis at room temperature.

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Section: Introductionmentioning

confidence: 94%

Section: ■ Introductionmentioning

confidence: 99%

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Tamtaji,

Kwon,

Musgrave

et al. 2024

ACS Appl. Mater. Interfaces

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“…SACs have displayed outstanding catalytic activity and selectivity in other electrochemical reactions, including HER [92][93][94] , OER [95][96][97] , ORR [98,99] , CO 2 RR [100,101] , etc., due to their 100% atomic utilization and strong interactions between active centers and matrices. Thanks to the merits, the SACs were also applied in the NRR and were supposed to adsorb and activate the inert N≡N bonds with high binding energy.…”

Section: Efficient Single Atom Electrocatalysts For Nrrmentioning

confidence: 99%

Recent progress in single atomic catalysts for electrochemical N₂ fixation

Fan,

Wang,

Liu

et al. 2024

Microstructures

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Ammonia (NH3), as an important chemical product, is industrially produced using the traditional energy-intensive Haber-Bosch method at high temperature and pressure. Electrochemical nitrogen reduction reaction (NRR) to synthesize NH3 at ambient conditions has been considered as a promising candidate for replacing Haber-Bosch process. However, major obstacles, such as poor catalytic activity and selectivity and extensive competitive hydrogen evolution reaction, remain in NRR, which urgently need to be addressed. Single atom electrocatalysts (SACs) have attracted wide attention in view of their nearly 100% atomic utilization and outstanding catalytic performance. In this review, recent theoretical and experimental advances on novel atomically dispersed electrocatalysts for NRR are summarized and highlighted. We start with the fundamental reaction mechanism of NRR. Then, different preparation methods and the strategies of boosting catalytic performance of SACs from the aspects of coordination environment, coordination number, metal-support interaction and spatial microenvironment regulation are presented and analyzed in detail. Following this, the extensive applications of SACs in terms of noble metal based-SACs and transition metal-based SACs in NRR are discussed. Finally, we provide a perspective of the challenges of SACs for NRR, aiming to guide the rational design of advanced NRR catalysts.

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Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

He,

Wang,

et al. 2024

Adv Funct Materials

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Electrocatalytic carbon dioxide reduction reaction (CO2RR) has been recognized as a promising route to convert carbon emissions to high‐value chemicals and fuels. Significant breakthroughs are usually inseparable from deeper understanding of reaction mechanisms. To this end, molecular dynamics (MD) simulations have been invaluable in providing detailed insights into elucidation of complex reaction pathways and prediction of overall electrochemical performance, thus bridging macroscopic experimental observations and microscopic explanatory mechanisms. Directed by MD simulations, tremendous efforts have been devoted toward enhancing the CO2RR with rational design of electrocatalyst and efficient construction of electrode/electrolyte interface. Herein, a comprehensive review of applications of MD simulations in CO2RR is emerged. To begin with, specific fundamentals along with familiar methods such as algorithm and force fields of various MD simulations have been summed up. Followed, employment of MD simulations in optimization of CO2RR is introduced, encompassing interpretation of electrocatalyst activity, explanation of electrolyte effect, and investigation of electrode microenvironment. Definitively, imminent challenges and avenues for optimization in future MD simulations are contemplated, envisioning this review as a guiding beacon for future endeavors aimed at harnessing MD simulations to propel CO2RR toward a realm of heightened efficiency, economic viability, and practical utility.

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Homonuclear multi-atom catalysts for CO₂ electroreduction: a comparison density functional theory study with their single-atom counterparts

Abstract: Multi-nuclear reaction centers on homonuclear multi-atom catalysts are designed to boost the CO2RR, outperforming their single-atom counterparts.

Cited by 7 publications

References 72 publications

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Recent progress in single atomic catalysts for electrochemical N₂ fixation

Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

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Homonuclear multi-atom catalysts for CO2 electroreduction: a comparison density functional theory study with their single-atom counterparts

Abstract: Multi-nuclear reaction centers on homonuclear multi-atom catalysts are designed to boost the CO2RR, outperforming their single-atom counterparts.

Cited by 7 publications

References 72 publications

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C3+) over Triple Atom Catalysts

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C3+) over Triple Atom Catalysts

Recent progress in single atomic catalysts for electrochemical N2 fixation

Molecular Dynamics Simulations for Electrocatalytic CO2 Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms

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Product

Resources

About

Homonuclear multi-atom catalysts for CO₂ electroreduction: a comparison density functional theory study with their single-atom counterparts

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Reaction Mechanism of Rapid CO Electroreduction to Propylene and Cyclopropane (C₃₊) over Triple Atom Catalysts

Recent progress in single atomic catalysts for electrochemical N₂ fixation

Molecular Dynamics Simulations for Electrocatalytic CO₂ Reduction: Bridging Macroscopic Experimental Observations and Microscopic Explanatory Mechanisms