Nickel polyphthalocyanine with electronic localization at the nickel site for enhanced CO2 reduction reaction

Chen, Kejun; Cao, Maoqi; Ni, Ganghai; Chen, Shanyong; Liao, Hanxiao; Zhu, Li; Li, Hongmei; Fu, Junwei; Hu, Junhua; Cortés, Emiliano; Liu, Min

doi:10.1016/j.apcatb.2022.121093

Cited by 79 publications

(53 citation statements)

References 55 publications

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“…No other gaseous products were detected by GC, because CO, as a two-electron product, is more easily generated than other four-, six-, or eight-electron products such as CH 3 OH and CH 4 , consistent with previous studies. [49,50] Moreover, no liquid products were produced, as evidenced by 1…”

Section: Electrocatalytic Activity Testmentioning

confidence: 99%

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Zhang

Mady

et al. 2022

ChemSusChem

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Developing highly efficient electrocatalysts for electrochemical CO2 reduction (ECR) to value‐added products is important for CO2 conversion and utilization technologies. In this work, a sulfur‐doped Ni−N−C catalyst is fabricated through a facile ion‐adsorption and pyrolysis treatment. The resulting Ni−NS−C catalyst exhibits higher activity in ECR to CO than S‐free Ni−N−C, yielding a current density of 20.5 mA cm−2 under −0.80 V versus a reversible hydrogen electrode (vs. RHE) and a maximum CO faradaic efficiency of nearly 100 %. It also displays excellent stability with negligible activity decay after electrocatalysis for 19 h. A combination of experimental investigations and DFT calculations demonstrates that the high activity and selectivity of ECR to CO is due to a synergistic effect of the S and Ni−NX moieties. This work provides insights for the design and synthesis of nonmetal atom‐decorated M−N−C‐based ECR electrocatalysts.

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Section: Electrocatalytic Activity Testmentioning

confidence: 99%

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Zhang

Mady

et al. 2022

ChemSusChem

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“…Among CO 2 reduction products, C 2 or multicarbon products have received extensive attention due to their higher energy density and application value. Copper (Cu)-based electrocatalysts are the star catalysts that can achieve carbon–carbon (C–C) coupling to generate C 2 or multicarbon products. − Though active site construction, ,,− grain facet/boundary regulation, − defects, ,, and the oxidation state ,, of Cu have been reported to enhance the activity and selectivity of C 2 or multicarbon products, optimizing the surface structure and properties of Cu catalysts to improve the C 2 product efficiency remains a hot topic and challenge. − …”

Section: Introductionmentioning

confidence: 99%

Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C₂ Hydrocarbons in the CO₂ Electroreduction

et al. 2022

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Electrocatalytic reduction of CO2 to multicarbon products is a potential strategy to solve the energy crisis while achieving carbon neutrality. To improve the efficiency of multicarbon products in Cu-based catalysts, optimizing the *CO adsorption and reducing the energy barrier for carbon–carbon (C–C) coupling are essential features. In this work, a strong local electric field is obtained by regulating the arrangement of Cu nanoneedle arrays (CuNNAs). CO2 reduction performance tests indicate that an ordered nanoneedle array reaches a 59% Faraday efficiency for multicarbon products (FEC2) at −1.2 V (vs RHE), compared to a FEC2 of 20% for a disordered nanoneedle array (CuNNs). As such, the very high and local electric fields achieved by an ordered Cu nanoneedle array leads to the accumulation of K+ ions, which benefit both *CO adsorption and C–C coupling. Our results contribute to the design of highly efficient catalysts for multicarbon products.

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“…A high current density is difficult to implement in the traditional H-type cell because of the limited mass transfer of CO 2 in an aqueous electrolyte. , CO 2 is supplied directly to the electrode by constructing a gas diffusion electrode in the flow cell, which surpasses the mass transfer of CO 2 in an aqueous electrolyte to enhance the performances of catalysts for eCO 2 RR . LSV curves of re-Bi NSs (Figure a) manifest that re-Bi NSs in the flow cell show higher current densities compared to those in the H-type cell.…”

Section: Resultsmentioning

confidence: 99%

“…The counter electrode was made of an IrO 2 -coated titanium sheet, and the reference electrode was an Ag/AgCl electrode. The electrolyte used in the test was 1 M KOH (pH = 14), and its flow rate was programmed at 30 mL min –1 in the cathode and anode compartments. , …”

Section: Methodsmentioning

confidence: 99%

Bismuth-Nanosheet-Based Catalysts with a Reconstituted Bi⁰ Atom for Promoting the Electrocatalytic Reduction of CO₂ to Formate

Xiao

et al. 2022

Ind. Eng. Chem. Res.

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The electrocatalytic reduction of CO2 shows significant potential for the conversion of CO2 to valuable chemicals and fuels. Herein, we develop a method for the preparation of two-dimensional Bi-based catalysts by the reconstitution of a Bi0 atom (re-Bi NSs). In situ Raman spectral analysis reveals that the reconstituted fresh Bi0 is the electrocatalytic active center, while BiIII is not. The as-prepared electrocatalyst exhibits excellent electrocatalytic activity for the generation of formate with a high faradaic efficiency (FEformate) of over 90% at an applied potential from −0.8 to −1.2 V versus reversible hydrogen electrode (RHE), with the corresponding j formate ranging from −13.76 to −44.89 mA cm–2. Moreover, the maximum FEformate reaches 94.6% at −1.0 V versus RHE with j formate of −32.2 mA cm–2. The catalyst also shows good long-term stability. The re-Bi NSs in a flow cell achieved a FEformate of 94.6% with a high current density of −400.0 mA cm–2. Our new strategy for the preparation of a catalyst with a reconstituted Bi0 atom will provide a novel tool for the design of highly active and stable Bi-based electrocatalysts.

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Nickel polyphthalocyanine with electronic localization at the nickel site for enhanced CO2 reduction reaction

Cited by 79 publications

References 55 publications

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C₂ Hydrocarbons in the CO₂ Electroreduction

Bismuth-Nanosheet-Based Catalysts with a Reconstituted Bi⁰ Atom for Promoting the Electrocatalytic Reduction of CO₂ to Formate

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Nickel polyphthalocyanine with electronic localization at the nickel site for enhanced CO2 reduction reaction

Cited by 79 publications

References 55 publications

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO2 Reduction with Near 100 % CO Selectivity

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO2 Reduction with Near 100 % CO Selectivity

Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C2 Hydrocarbons in the CO2 Electroreduction

Bismuth-Nanosheet-Based Catalysts with a Reconstituted Bi0 Atom for Promoting the Electrocatalytic Reduction of CO2 to Formate

Contact Info

Product

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Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Sulfur‐Decorated Ni−N−C Catalyst for Electrocatalytic CO₂ Reduction with Near 100 % CO Selectivity

Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C₂ Hydrocarbons in the CO₂ Electroreduction

Bismuth-Nanosheet-Based Catalysts with a Reconstituted Bi⁰ Atom for Promoting the Electrocatalytic Reduction of CO₂ to Formate