Highly efficient ammonia synthesis at low temperature over a Ru–Co catalyst with dual atomically dispersed active centers

Peng, Xuanbei; Liu, Han-Xuan; Zhang, Yangyu; Huang, Zheng-Qing; Yang, Linlin; Jiang, Yafei; Wang, Xiuyun; Zheng, Lirong; Chang, Chun‐Ran; Au, Chak Tong; Jiang, Lilong; Li, Jun

doi:10.1039/d1sc00304f

Cited by 39 publications

(17 citation statements)

References 78 publications

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“…[ 7–10 ] In recent years, Co single atom catalysts (SACs), as one of the most emerging kinds of heterogeneous catalysts, possess special electronic structure, utmost Co atom utilization efficiency, and uniformly isolated Co active sites. [ 11–17 ] Such unique properties make Co SACs an attractive platform to bridge the gap between homogeneous and heterogeneous PMS activation. [ 1,11,17–20 ]…”

Section: Introductionmentioning

confidence: 99%

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Dong

Chen

Tang

et al. 2022

Adv Funct Materials

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Single atom catalysts (SACs) have been growing as an emerging "hot" topic in environmental remediation. Their performance can be rationally optimized via modulating spatial coordination configuration and the porous structure of SACs, which is still challenging. Herein, a novel Si, N co-coordinated cobalt SAC (p-CoSi 1 N 3 @D) with 3D free standing architecture is tailored via employing natural mineral (diatomite) as a Si source and porous template. Theoretical calculations and experimental analysis reveal that the substitution of N by Si dramatically accelerates the interaction and electron transfer between peroxymonosulfate and the Co single atom center. Moreover, p-CoSi 1 N 3 @D inherits the hierarchically porous architecture of diatomite, providing more accessible cobalt sites and open diffusion channels for peroxymonosulfate and contaminants in water treatment applications. Thanks to optimal coordination structure and porous architecture, p-CoSi 1 N 3 @D can serve as a highly active catalyst for peroxymonosulfate activation, with a turnover frequency of 299.8 min −1 for bisphenol A degradation, surpassing those of catalysts with transition metal SACs or oxides in the disclosed literature. This work provides a novel strategy for the development of SACs for wastewater reclamation, and deepens the understanding of the significant role of templates in spatial coordination configuration of SACs.

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Section: Introductionmentioning

confidence: 99%

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Dong

Chen

Tang

et al. 2022

Adv Funct Materials

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“… 9 , 11 With the efforts of researchers and scientists, different kinds of efficient NRR electrocatalysts have already been produced to accelerate the NRR process. 12 − 14 However, a significant challenge of increasing the concentration of N 2 gas in the solution needs to be overcome due to a relatively high kinetic barrier occurring at the solid–liquid–gas interface in the NRR process. 15 Hence, the electrochemical synthesis of NH 3 using N 2 as a nitrogen source has a broad prospect, but there is still a long way to go to obtain considerable NH 3 yield in practical application.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Evaluation of Electrochemical Nitrate Reduction Reaction on Graphdiyne-Supported Transition Metal Single-Atom Catalysts

Wang

2022

ACS Omega

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The electrochemical reaction can be applied as a powerful method to eliminate the pollution of nitrate (NO 3 – ) and as a feasible synthesis to enable the conversion of nitrate into ammonia (NH 3 ) at room temperature. Herein, density functional theory calculations are applied to comprehensively analyze the electrochemical nitrate reduction reaction (NO 3 RR) on graphdiyne-supported transition metal single-atom catalysts (TM@GDY SACs) for the first time. It can be found that the vanadium-anchored graphdiyne (V@GDY) displays the lowest limiting potential of −0.63 V versus a reversible hydrogen electrode among the investigated systems in this work. Notably, the competing hydrogen evolution reaction is relatively restrained due to the comparatively weak adsorption of the H proton on the TM@GDY SACs. Moreover, higher energy intake is needed to overcome the energy barrier during the formation of byproducts (NO 2 , NO, N 2 O, and N 2 ) on V@GDY without applying extra electrode potential, showing the selectivity of NH 3 in the NO 3 RR process. The ab initio molecular dynamics simulation denotes that the V@GDY possesses excellent structure stability at the temperature of 600 K without much distortion, compared with the initial shape, indicating the promise for synthesis. This study not only offers a feasible NO 3 RR electrocatalyst but also paves the way for the development of the NO 3 RR process.

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“…The RuCo DACs reported by Peng et al. can realize the conversion of nitrogen to ammonia under mild conditions (400 °C, 1 MPa) [114] . The authors claimed that the addition of Ru to single‐site Co caused a significant overlapping of Co t 2g and e g orbitals and gave rise to a “free” Co atom, which acted as a bridge to the electron transfer from pyrrolic N to Ru atom, then to N 2 .…”

Section: Heteronuclear Dacs With Two Different Metal Atomsmentioning

confidence: 99%

Synergetic Dual‐Atom Catalysts: The Next Boom of Atomic Catalysts

Liu

Rong

Zhang³

2022

ChemSusChem

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Dual‐atom catalysts (DACs) are an important branch of single‐atom catalysts (SACs), in which the former can effectively break the dilemma faced by the traditional SACs. The synergetic effects between bimetallic atoms provide many active sites, promising to improve catalytic performance and even catalyze more complex reactions. This paper reviews the recent research progresses of two kinds of DACs, including homonuclear and heteronuclear DACs, and their applications in oxygen reduction, carbon dioxide reduction, hydrogen evolution, oxygen evolution, Zn‐air batteries, tandem catalytic reactions, and so on. In addition, in order to promote the further development of DACs, the challenges and perspectives of DACs are put forward.

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Highly efficient ammonia synthesis at low temperature over a Ru–Co catalyst with dual atomically dispersed active centers

Abstract: The desire of a carbon-free society and the continuously increasing demand of clean energy make it valuable to exploit green ammonia (NH3) synthesis that proceeds via electrolysis driven Haber-Bosch (eHB)...

Cited by 39 publications

References 78 publications

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Mineral Modulated Single Atom Catalyst for Effective Water Treatment

Theoretical Evaluation of Electrochemical Nitrate Reduction Reaction on Graphdiyne-Supported Transition Metal Single-Atom Catalysts

Synergetic Dual‐Atom Catalysts: The Next Boom of Atomic Catalysts

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