Discovery of main group single Sb–N<sub>4</sub> active sites for CO<sub>2</sub> electroreduction to formate with high efficiency

Jiang, Zhuoli; Wang, Tao; Pei, Jiajing; Shang, Huishan; Zhou, Danni; Li, Haijing; Dong, Juncai; Wang, Yu; Cao, Rui; Zhuang, Zhongbin; Chen, Wenxing; Wang, Dingsheng; Zhang, Jiatao; Li, Yadong

doi:10.1039/d0ee01486a

Cited by 263 publications

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“…Jiang et al demonstrated that the formation HCOO* via the first proton–electron pair addition is more favorable than *COOH formation by DFT calculations, so the major product is formate of Sb SACs which consisted of Sb–N 4 anchored on N‐doped carbon nanosheets. [ 84 ] This catalyst can serve ECR to produce formate with FE of 94.0% at −0.8 V versus RHE. Shang et al designed In SACs containing exclusive isolated In δ+ ‐N 4 sites on N‐doped carbon matrix derived metal–organic frameworks (MOFs).…”

Section: Regulating Central Atoms For Improving the Performance Of Sacsmentioning

confidence: 99%

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

et al. 2020

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Excessive consumption of fossil fuels gives rise to the increasing emission of carbon dioxide (CO2) in the atmosphere and furthers the ecocrisis. Electrochemical CO2 reduction (ECR) has both functions of dwindling greenhouse gas concentration and converting it into valuable products. Due to the intrinsic chemical inertness of CO2 molecules, the study on efficient and low‐cost catalysts has attracted much attention. Recently isolated atoms, dispersed in stable support, play an important role in decreasing energy barriers of intermediate steps and obtaining target products with high activity and selectivity for ECR. The effective regulation of central atoms or coordination environment is significant to realize the desired performances of ECR with a high efficiency and selectivity. Hence, a comprehensive summary about strategies for improving the performance of ECR on single atom catalysts (SACs) is necessary. Herein, the SACs on various supports are introduced, the methods to design stable SACs are discussed, and the strategies for tuning the performance of ECR on SACs are summarized. The localized environment manipulation is widely used for high‐performance SACs design, including regulating central atoms and coordination environment. Finally, the perspectives are discussed to shed light on the rational design of intriguing SACs for ECR.

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Section: Regulating Central Atoms For Improving the Performance Of Sacsmentioning

confidence: 99%

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

et al. 2020

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“…DFT calculations confirmed that the exclusive Sb δ + -N 4 sites is the active site for electrocatalytic reduction of CO 2 . [29] In addition, the local coordination structure can be regulated by changing conditions such as carbon support or temperature to improve the performance of the catalyst. Pan et al have used the N-coordination strategy to synthesize an atomically dispersed Co-N 5 active site with a template of hollow nitrogen doped porous carbon spheres (HNPCSs).…”

Section: Introductionmentioning

confidence: 99%

The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO₂ Electroreduction

et al. 2020

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Single-atom metal and nitrogen co-doped carbon catalysts have caused an extensive research boom for electrochemical CO 2 reduction reaction (CO 2 RR). The diversity of metal-N coordination environment at high temperature limits the accurate study of electrocatalytic active sites. In this work, Fe porphyrin is anchored on a nitrogen-doped graphene substrate through the coordination between Fe and N atoms to form atomically dispersed Fe and N co-doped graphene nanosheets. The confinement anchoring effect of the nitrogen-doped graphene substrate prevents Fe atoms from agglomerating into Fe nanoparticles. Apart from that, the different Fe-N coordination environments and their catalytic effects on CO 2 RR are investigated by temperature changes. Electrochemical tests and density functional theory (DFT) calculations indicate that the atomically dispersed saturated Fe-N coordination catalyst have excellent performance for CO2RR and the Faradaic efficiency towards CO can up to 97 % at a potential of À 0.5 V (vs. reversible hydrogen electrode, RHE).

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“…As illustrated in Equations (1)(2)(3)(4)(5)(6)(7)(8)(9)(10)(11)(12), different reduction potentials are required to obtain different reduction products for CO 2 RR. Experimentally, researchers tend to define the onset potential as the potential where the products of ECO 2 RR can be firstly detectable.…”

Section: Onset Potential and Overpotentialmentioning

confidence: 99%

“…For example, main‐group metals such as Bi, In, Sb, and Sn are efficient for ECO 2 RR toward formate production. [ 12 ] TMs such as Fe, Co, Ni, Cu, and Zn become the most popular elements studied in ECO 2 RR for the high FE, current density, and selectivity of numerous products. [ 13 ] Among them, Co‐based catalysts are strikingly efficient for the production of CO and HCOOH in ECO 2 RR ( Figure ).…”

Section: Introductionmentioning

confidence: 99%

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

Chen

Zhang

et al. 2020

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million (ppm), which is ≈50% higher than that of the pre-industrial level (280 ppm). [1] The consequent climate change (the average temperature increase of 0.8 °C above the pre-industrial level) causes global warming, one of the top environmental concerns. [2] To maintain the sustainable development of the society, the Intergovernmental Panel on Climate Change (IPCC) recently recommended the warming limit to 1.5 °C rather than 2.0 °C to reduce catastrophic climate change issues, requiring the commitment to take action to control global carbon emission. [3] Under the Paris Agreement, many countries endeavor to reduce greenhouse gas emissions gradually by 2030. [4] The carbon capture and storage (CCS) is a feasible strategy to lower the CO 2 emissions substantially. Long-term storage issues related to the leakage of CO 2 and the lack of economic incentives limited its development. [5] The CO 2 reduction reactions (CO 2 RR) that convert CO 2 into other value-added carbon products could provide a well alternative to the utilization of the captured CO 2 , which not only contributes to the mitigation of CO 2 emission but also offers useful products that can serve as fuels such as CO, HCOOH, CH 3 OH, and CH 4. [6] Moreover, the drive power of CO 2 RR could come from renewable energy resources, such as solar, wind, and hydraulic resources, which indicates that in a green concept, CO 2 RR could complete the carbon loop and potentially solve the issues of global warming and energy crisis simultaneously. [7] 1.1. Fundamental Reaction Pathways of CO 2 RR CO 2 RR is not thermodynamically and kinetically favorable. Every reduction pathway demands a certain amount of energy input. Equations (1-13) shows the reaction steps involved in CO 2 RR (in pH = 7 aqueous solution, vs Normal Hydrogen Electrode (NHE)). [8] As illustrated, it requires a significant amount of reorganizational energy between the linear molecule CO 2 and the bent radical anion − CO 2 • (Equation (1)). When coupling with proton in the reaction, the required reaction energy decreases (Equations (2-12)). Aqueous media with H 2 O molecules become ideal for providing proton into the CO 2 RR system. The reduction potential of hydrogen evolution reaction (HER) (Equation (13)) is close to that of CO 2 RR. It makes HER a competitive reaction against CO 2 RR during the reduction CO 2 reduction reaction (CO 2 RR) provides a promising strategy for sustainable carbon fixation by converting CO 2 into value-added fuels and chemicals. In recent years, considerable efforts are focused on the development of transition-metal (TM)-based catalysts for the selectively electrochemical CO 2 reduction reaction (ECO 2 RR). Co-based catalysts emerge as one of the most promising electrocatalysts with high Faradaic efficiency, current density, and low overpotential, exhibiting excellent catalytic performance toward ECO 2 RR for CO and HCOOH productions that are economically viable. The intrinsic contribution of Co and the synergistic effects in Co-hybrid catalysts play essential roles for ...

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Discovery of main group single Sb–N₄ active sites for CO₂ electroreduction to formate with high efficiency

Abstract: Main group antimony (Sb) species are promising electrocatalysts that promote CO2 reduction reaction (CO2RR) to formate, which is an important hydrogen storage material and a key chemical intermediate in many...

Cited by 263 publications

References 67 publications

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO₂ Electroreduction

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives

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Discovery of main group single Sb–N4 active sites for CO2 electroreduction to formate with high efficiency

Abstract: Main group antimony (Sb) species are promising electrocatalysts that promote CO2 reduction reaction (CO2RR) to formate, which is an important hydrogen storage material and a key chemical intermediate in many...

Cited by 263 publications

References 67 publications

Recent Advances in Strategies for Improving the Performance of CO2 Reduction Reaction on Single Atom Catalysts

Recent Advances in Strategies for Improving the Performance of CO2 Reduction Reaction on Single Atom Catalysts

The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO2 Electroreduction

Nanostructured Cobalt‐Based Electrocatalysts for CO2Reduction: Recent Progress, Challenges, and Perspectives

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Discovery of main group single Sb–N₄ active sites for CO₂ electroreduction to formate with high efficiency

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

Recent Advances in Strategies for Improving the Performance of CO₂ Reduction Reaction on Single Atom Catalysts

The Effect of the Coordination Environment of Atomically Dispersed Fe and N Co‐doped Carbon Nanosheets on CO₂ Electroreduction

Nanostructured Cobalt‐Based Electrocatalysts for CO₂Reduction: Recent Progress, Challenges, and Perspectives