Typical transition metal single-atom catalysts with a metal-pyridine N structure for efficient CO2 electroreduction

Cai, Weiping; Hu, Xiangming; Hu, Xiaosong; Liu, Xinyu; Guan, Qingxin; Hao, Ran; Liu, Yuping; Li, Wei

doi:10.1016/j.apcatb.2021.120331

Cited by 56 publications

(30 citation statements)

References 57 publications

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“…[ 196 ] Among many reduction products, the CO (or syngas) is considered to be one of the most ideal and economical raw material in subsequent chemical synthesis of diversified organic products. [ 197 ] However, CO 2 reduction reaction is a multielectron process from perspective of kinetics, and products are complex, where catalyst is the key to achieve efficient selective CO 2 reduction. [ 198 ] Single‐atom metal electrocatalysts with a specific coordination environment, especially the atomically dispersed transition metal on N‐doped carbon (M–N–C), are widely used in electrocatalytic CO 2 reduction due to their maximum atomic utilization, ultrahigh metal content, excellent activity, and selectivity (see Figure and Table 4 for details).…”

Section: Heterogeneous Catalysis Applications Of Afcsmentioning

confidence: 99%

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Liao

et al. 2022

Small Structures

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In recent years, single‐atom catalysts (SACs) with high metal loading have emerged in different heterogeneous catalysis fields and shown extraordinary catalytic properties. When there are enough coordination atoms (or functional groups) on the supports, it is possible to achieve a limit monolayer atom loading on the surface of supports with ultrahigh atom density (5–15 atoms nm−2) and extremely close site distance (0.2–0.5 nm), by using appropriate synthesis methods and procedures. These high‐density metal atoms usually have no or less metal bonds, which are mostly isolated by support atoms to form 3D foam‐like atomic constructions. Herein, a new notion of metal atomic foam catalysts (AFCs) is propsed to redefine these ultrahigh‐density SACs accommodated by specific supports. This new paradigm of 3D atomic construction for SACs has potential significance for both theoretical research and industrial applications. The latest major advancements in the controllable synthesis of AFCs on various supports (e.g., polymer, carbon, and metallic compound) via different methods (bottom‐up or top‐down approaches) are summarized. The latent catalytic principles and typical application cases of AFCs are emphasized in a wide range of heterogeneous catalysis fields (e.g., thermocatalysis, photocatalysis, electrocatalysis, etc.). The challenges and prospects of this newly 3D ultrahigh‐density AFCs materials in practical industrial application are pointed out as well.

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Section: Heterogeneous Catalysis Applications Of Afcsmentioning

confidence: 99%

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Liao

et al. 2022

Small Structures

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“…Recently, single-atom catalysts (SACs) have attracted tremendous interest in ECR due to their maximum metal utilization efficiency and uniform atomic active sites, in which three atomically dispersed metals (Ni, Fe, and Co) and nitrogen codoped carbon (M-N-C) materials with MN x active sites have been widely studied owing to their extraordinary activity and low cost in CO 2 reduction to CO. ,, In theory, compared with NiN 4 and FeN 4 sites, CoN 4 sites show an optimum balance between the energy barriers for *COOH formation and CO desorption, , while the reported Co-N-C with CoN 4 sites often exhibits poor selectivity and activity for ECR. − To this end, the strategies of constructing integrated electrodes and adjusting the coordination number were adopted to improve the ECR performance of Co-N-C. ,, Even so, it is still a challenge to prepare a Co-N-C electrocatalyst using a simple method to achieve both high CO faradic efficiency (FE CO ) and CO current density at low overpotentials.…”

Section: Introductionmentioning

confidence: 99%

Diminishing the Uncoordinated N Species in Co-N-C Catalysts toward Highly Efficient Electrochemical CO₂ Reduction

et al. 2022

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Atomically dispersed metal and nitrogen codoped carbon (M-N-C) catalysts with N-coordinated metal (MN x ) sites have shown compelling performance in electrochemical CO 2 reduction (ECR). However, extra uncoordinated N species commonly coexist with MN x sites in M-N-C, which are impossible to ignore due to their inevitable interference in catalytic performance. Considering this, we developed high-performance Co-N-C for ECR by diminishing the uncoordinated N species. The resulting electrocatalyst displays a CO faradic efficiency (FE CO ) of 99.4% with a CO current density of −24.8 mA•cm −2 at a low overpotential of 0.49 V in an H-type cell, and a high FE CO over 90% is obtained in a flow cell within a wide current density window (50−600 mA•cm −2 ), exceeding all reported Co-N-C catalysts. Density functional theory calculations reveal that isolated CoN 4 sites can reduce the energy barrier required for the formation of COOH* and suppress the occurrence of hydrogen evolution compared with CoN 4 sites with extra uncoordinated N species, thus resulting in enhanced activity and selectivity in CO production.

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“…Similarly, a high concentration of pyridinic nitrogen species has been shown to promote CO 2 reduction, hypothesized to be through offering an abundance of chemisorption sites. [24,25] For the CO-specific catalysts, the series of FeMoÀ NÀ C catalysts shows an increase in this ratio compared to the mono-and bi-metallic catalysts synthesized at higher temperatures (975/950), which suggests a more favorable local chemical environment for CO 2 reduction (Table S4).…”

Section: Synthesis/characterization Of Atomically Dispersed Metal-nit...mentioning

confidence: 98%

Synergistic Electrocatalytic Syngas Production from Carbon Dioxide by Bi‐Metallic Atomically Dispersed Catalysts

et al. 2022

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The production of syngas by traditional processes such as steam methane reforming is energetically intensive and produces a large amount of CO2 emissions. In contrast, the electrochemical CO2 reduction reaction (CO2RR) enables the carbon neutral production of syngas at ambient conditions. Among non‐precious metal catalysts, metal‐nitrogen‐carbon electrocatalysts are inexpensive and highly selective towards syngas production. This study examined the selectivity of mono‐ and bi‐metallic (M−N−C, M=Fe, Mo or FeMo) electrocatalysts towards syngas production. The ratio of the CO : H2 in the syngas was tuned by modifying the ratio of the metallic precursors in the bi‐metallic FeMo−N−C catalysts, tailoring the catalysts’ selectivity towards the CO2RR or the hydrogen evolution reaction (HER). The catalyst synthesis temperature(s) were considered as they influence the catalyst morphology and activity. Further, the dependence of the ratio of CO : H2 in the syngas as a function of the potential was explored for the different bi‐metallic catalysts. This work showed that by tailoring both the ratio of Fe : Mo in the bi‐metallic catalyst and optimizing the reductive potential, a CO : H2 ratio between 0.25 to 5 was achievable. This study demonstrated a novel approach in which the ratio of the product syngas composition could be tailored in a single reaction, without the need for further downstream processing to reach a desired composition.

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Typical transition metal single-atom catalysts with a metal-pyridine N structure for efficient CO2 electroreduction

Cited by 56 publications

References 57 publications

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Diminishing the Uncoordinated N Species in Co-N-C Catalysts toward Highly Efficient Electrochemical CO₂ Reduction

Synergistic Electrocatalytic Syngas Production from Carbon Dioxide by Bi‐Metallic Atomically Dispersed Catalysts

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Typical transition metal single-atom catalysts with a metal-pyridine N structure for efficient CO2 electroreduction

Cited by 56 publications

References 57 publications

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Emerging Ultrahigh‐Density Single‐Atom Catalysts for Versatile Heterogeneous Catalysis Applications: Redefinition, Recent Progress, and Challenges

Diminishing the Uncoordinated N Species in Co-N-C Catalysts toward Highly Efficient Electrochemical CO2 Reduction

Synergistic Electrocatalytic Syngas Production from Carbon Dioxide by Bi‐Metallic Atomically Dispersed Catalysts

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Diminishing the Uncoordinated N Species in Co-N-C Catalysts toward Highly Efficient Electrochemical CO₂ Reduction