Coordination environment engineering to boost electrocatalytic CO2 reduction performance by introducing boron into single-Fe-atomic catalyst

Liu, Shuai; Jin, Mengmeng; Sun, Jiaqiang; Qin, Yongji; Gao, Sanshuang; Chen, Yu; Zhang, Shusheng; Luo, Jun; Liu, Xijun

doi:10.1016/j.cej.2022.135294

Cited by 97 publications

(57 citation statements)

References 67 publications

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“…[11] Benefited from these advantages, SACs have been extensively applied in electrocatalytic reactions, such as ORR, [16][17][18] OER, [19][20][21] and CO 2 RR. [22][23][24] Although SACs exhibit particular advantages, some intrinsic defects limit their further development: (1) when it comes to complex processes involving multiple reactive intermediates, all of them are adsorbed on the same active center. The single adsorption site cannot achieve the optimal adsorption state for all intermediates, which lowers the selectivity toward target products.…”

Section: Introductionmentioning

confidence: 99%

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Jiang

Cheng

et al. 2022

Small Methods

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Atomically dispersed metal catalysts have been widely used in electrocatalysis because of their outstanding catalytic activity and high atomic utilization efficiency. As an extension of single‐atom catalysts (SACs), dual‐atom catalysts (DACs) provide new insights for the development of atomic‐scale catalysts. Higher metal loading and more flexible active sites endow DACs with improved catalytic performance as well as optimized reaction mechanism model. In this review, DACs are firstly classified according to their configurations and metal sites. Subsequently, the synthetic strategies and characterization techniques of DACs are introduced. Furthermore, the applications of DACs are exemplified in various electrocatalytic reactions, including oxygen reduction reaction, oxygen evolution reaction and carbon dioxide reduction reaction. Finally, the prospects to be expected and challenges to be faced with are discussed.

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Section: Introductionmentioning

confidence: 99%

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Jiang

Cheng

et al. 2022

Small Methods

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“…Accordingly, great efforts have been made to develop an eco-friendly and cost-effective route for C2H4 production. In this regard, the electrocatalytic CO2 reduction (ECR) to C2H4 under ambient conditions offers a promising pathway to replace the industrial steam cracking process [4][5][6][7][8][9][10] , which enables to use renewable energies and also reduces anthropogenic CO2 emissions [11][12][13][14] . However, the chemical inert of CO2 molecule and multielectron transfer processes involved in the ECR-to-C2H4 hinder the economic feasibility of this proposed conversion process 6,7,15 .…”

Section: Introductionmentioning

confidence: 99%

Oxygen Vacancy-Rich Amorphous Copper Oxide Enables Highly Selective Electroreduction of Carbon Dioxide to Ethylene

Wei¹,

Zhang²,

Liu³

et al. 2022

Acta Physico Chimica Sinica

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The ever-increasing carbon dioxide (CO2) emissions caused by excessive fossil fuel consumption induce environmental issues such as global warming. To overcome this, the electrocatalytic CO2 reduction (ECR) under ambient conditions offers an appealing approach for converting CO2 to value-added chemicals and realizing a closed carbon loop. Among the ECR products, ethylene (C2H4), an important building block for plastics and other chemicals, has attracted considerable attention owing to its compatibility with existing infrastructure and the promising substitution of industrial steam cracking. In recent years, numerous efforts have been devoted to developing highly active and selective catalysts for converting CO2 to C2H4, with most studies having focused on Cu-based materials. Despite the significant advancements made to date, the development of the ECR-to-C2H4 process is still hindered by the lack of suitable catalysts that can effectively activate CO2 and strengthen the surface binding of *CO and *COH species. In this study, an amorphous copper oxide (CuOx) nanofilm that is rich in oxygen vacancies was prepared via a facile vacuum evaporation method for the efficient electrocatalytic conversion of CO2 to C2H4. It was expected that the nano-scale electrode thickness would greatly accelerate charge-and mass-transfer during CO2 electrolysis. Moreover, the introduction of oxygen vacancies favored the adsorption of CO2 and intermediates. As a result, in a typical H-cell, the synthesized defective catalyst delivered a maximum Faradaic efficiency of 85 ± 3% at −1.3 V versus the reversible hydrogen electrode and maintained a stable C2H4 selectivity over 48 h in a 0.1 M potassium bicarbonate solution. Interestingly, the performance observed with the synthesized electrocatalyst in this study is comparable with that of state-of-the-art Cu-based ECR catalysts. Additional structural and chemical characterizations confirmed the robust nature of the as-prepared catalyst. Moreover, when the catalyst was utilized in a membrane electrode assembly cell, it achieved a maximum C2H4 partial current density of approximately 115.4 mA•cm 2 at a cell voltage of −1.95 V and Faradaic efficiency of 78 ± 2% at a cell voltage of −1.75 V. Furthermore, theoretical and experimental analyses revealed that oxygen defects not only favored CO2 adsorption but also enabled strong affinities for *CO and *COH intermediates, which synergistically contributed to a high selectivity for C2H4 formation. We believe that our present work will motivate the exploration of amorphous Cu-based materials for achieving efficient CO2-to-C2H4 electrolysis and be a guide towards fundamentally understanding the mechanism of catalytic CO2 reduction.

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“…Besides, most of the Sn-based ECR catalysts are powders, which are typically deposited onto conductive substrates with polymer binders, resulting in limited exposed active sites. 16,17 Therefore, it would be a significant step forward to prepare a large-scale and binder-free ECR Sn-based catalyst with high formate selectivity in high current density electrolysis. 18,19 Herein, we report a polycrystalline SnS x (p-SnS x ) nanofilm deposited on carbon paper via a simple vacuum evaporation method.…”

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confidence: 99%

“…32 Overall, the combination of metallic Sn and residual sulfide collectively contributes to an enhanced ECR activity toward formate formation. For industrial applications, 17,19,29,33 the ECR performance of p-SnS x was further investigated in a 5 cm 2 MEA electrolyzer (Fig. 4a).…”

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Polycrystalline SnS_x nanofilm enables CO₂ electroreduction to formate with high current density

et al. 2022

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Coordination environment engineering to boost electrocatalytic CO2 reduction performance by introducing boron into single-Fe-atomic catalyst

Cited by 97 publications

References 67 publications

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Oxygen Vacancy-Rich Amorphous Copper Oxide Enables Highly Selective Electroreduction of Carbon Dioxide to Ethylene

Polycrystalline SnS_x nanofilm enables CO₂ electroreduction to formate with high current density

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Coordination environment engineering to boost electrocatalytic CO2 reduction performance by introducing boron into single-Fe-atomic catalyst

Cited by 97 publications

References 67 publications

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Recent Advances in Dual‐Atom Site Catalysts for Efficient Oxygen and Carbon Dioxide Electrocatalysis

Oxygen Vacancy-Rich Amorphous Copper Oxide Enables Highly Selective Electroreduction of Carbon Dioxide to Ethylene

Polycrystalline SnSx nanofilm enables CO2 electroreduction to formate with high current density

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Polycrystalline SnS_x nanofilm enables CO₂ electroreduction to formate with high current density