Active-site and interface engineering of cathode materials for aqueous Zn—gas batteries

Liu, Wenxian; Feng, Jinxiu; Wei, Tianran; Liu, Qian; Zhang, Shusheng; Luo, Ying; Luo, Jun; Liu, Xijun

doi:10.1007/s12274-022-4929-7

Cited by 75 publications

(60 citation statements)

References 247 publications

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“…The Gibbs free energy and structural configuration of electrochemical CO 2 reduction into CO were given in Figure 6b and Figure S8, respectively. For all the models, the formation of *COOH is the rate‐determining step, which is consistent with the previous reports [30,33,34] . We first compared the C and N (Figure S9) sites in NC for CO 2 R, and confirmed that the C atom adjacent to graphitic N are active sites in NC, with the free energy barrier for *COOH formation of 2.01 eV.…”

Section: Resultssupporting

confidence: 89%

“…For all the models, the formation of *COOH is the rate-determining step, which is consistent with the previous reports. [30,33,34] We first compared the C and N (Figure S9) sites in NC for CO 2 R, and confirmed that the C atom adjacent to graphitic N are active sites in NC, with the free energy barrier for *COOH formation of 2.01 eV. The results also accord with the reports of Zhang et al [24] Compared with NC, NC@Ag and Ag@NC both show lower free energy barriers for CO 2 R (1.33 eV for NC@Ag and 0.48 eV for Ag@NC).…”

Section: Chemelectrochemmentioning

confidence: 99%

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Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

et al. 2022

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Electrochemical CO 2 reduction is an environmentally sustainable way for CO 2 conversion and utilization, the development of which needs highly efficient catalysts. Ag-based materials are one kind of electrocatalyst that are catalytically active for CO 2 reduction to CO. In this work, Ag clusters were fabricated on nitrogen-doped porous carbon nanomaterials by a hightemperature annealing method. The well-dispersion of Ag sites on nitrogen-doped carbons (Ag/NC) promoted CO production. As a result, Ag/NC showed a maximum Faradaic efficiency of 94 % at À 0.7 V versus reversible hydrogen electrode (vs RHE) at room temperature. In addition, Ag/NC showed good CO 2 reduction stability, and the CO Faradaic efficiency remained stable at about 90 % at À 0.7 V vs RHE for 12 h. Density functional theory calculation indicated that the cooperation of Ag and N-dopings effectively reduced the activation energy barrier of CO 2 reduction relative to hydrogen evolution reaction and thus effectively promoted the electrocatalytic reduction of CO 2 molecules to CO. This method provides a new idea for the synthesis of CO 2 reduction catalysts with higher activity, selectivity and stability.

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Section: Resultssupporting

confidence: 89%

Section: Chemelectrochemmentioning

confidence: 99%

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

et al. 2022

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“…In the anode chamber, HMF oxidation occurred; while for the cathode chamber, hydrogen product was generated. 37,38 Fig. 4e shows the LSV curves taken at 5 mV s À1 .…”

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confidence: 99%

A dual-functional Bi-doped Co₃O₄ nanosheet array towards high efficiency 5-hydroxymethylfurfural oxidation and hydrogen production

et al. 2023

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“…Thus, the co-existence of Cu + and Vo synergistically contributes stronger affinities to *CO and *COH, which can optimize the C2H4 pathway 4 . Therefore, this inspires us to seek a catalyst with abundant Cu + and Vo species by employing the atomic regulation strategy [19][20][21][22][23][24][25][26][27] , which is considered to be active for C2H4 production.…”

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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Active-site and interface engineering of cathode materials for aqueous Zn—gas batteries

Cited by 75 publications

References 247 publications

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

A dual-functional Bi-doped Co₃O₄ nanosheet array towards high efficiency 5-hydroxymethylfurfural oxidation and hydrogen production

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

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Active-site and interface engineering of cathode materials for aqueous Zn—gas batteries

Cited by 75 publications

References 247 publications

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO2 Reduction

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO2 Reduction

A dual-functional Bi-doped Co3O4 nanosheet array towards high efficiency 5-hydroxymethylfurfural oxidation and hydrogen production

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

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Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

Nitrogen Defects in Porous Carbons with Adjacent Silver Nanoclusters for Efficient CO₂ Reduction

A dual-functional Bi-doped Co₃O₄ nanosheet array towards high efficiency 5-hydroxymethylfurfural oxidation and hydrogen production