Simultaneous Achieving of High Faradaic Efficiency and CO Partial Current Density for CO<sub>2</sub> Reduction via Robust, Noble‐Metal‐Free Zn Nanosheets with Favorable Adsorption Energy

Liu, Kaihua; Wang, Jiazhi; Shi, Ming; Yan, Jun‐Min; Jiang, Qing

doi:10.1002/aenm.201900276

Cited by 104 publications

(100 citation statements)

References 53 publications

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“…Zinc is a CO‐producing metal for CO 2 RR. Various nanostructured Zn catalysts have been constructed to convert CO 2 to CO, such as porous Zn catalysts, [ 133,134 ] Zn nanoparticles, [ 135 ] Zn nanosheet, [ 136 ] and Zn dendrites. [ 137 ] Similar to its metal/oxide counterparts, single‐atom Zn catalysts have also been reported to convert CO 2 into CO through CO 2 RR.…”

Section: Heterogeneous Single‐atom Catalysts For Co2rr To Co Productmentioning

confidence: 99%

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

et al. 2020

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The electrochemical CO2 reduction reaction (CO2RR) is of great importance to tackle the rising CO2 concentration in the atmosphere. The CO2RR can be driven by renewable energy sources, producing precious chemicals and fuels, with the implementation of this process largely relying on the development of low‐cost and efficient electrocatalysts. Recently, a range of heterogeneous and potentially low‐cost single‐atom catalysts (SACs) containing non‐precious metals coordinated to earth‐abundant elements have emerged as promising candidates for the CO2RR. Unfortunately, the real catalytically active centers and the key factors that govern the catalytic performance of these SACs remain ambiguous. Here, this ambiguity is addressed by developing a fundamental understanding of the CO2RR‐to‐CO process on SACs, as CO accounts for the major product from CO2RR on SACs. The reaction mechanism, the rate‐determining steps, and the key factors that control the activity and selectivity are analyzed from both experimental and theoretical studies. Then, the synthesis, characterization, and the CO2RR performance of SACs are discussed. Finally, the challenges and future pathways are highlighted in the hope of guiding the design of the SACs to promote and understand the CO2RR on SACs.

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Section: Heterogeneous Single‐atom Catalysts For Co2rr To Co Productmentioning

confidence: 99%

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

et al. 2020

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“…Because the dissociative CO2 binding energy of CO2 •−* by oxidative LSV experiments in 0.1 M KOH electrolyte. [59][60][61] As shown in Figure S16, Ni-N4/C-NH2 demonstrates a negative potential of OH − adsorption than that of Ni-N4/C, evidencing a stronger adsorption strength of OH − on catalyst surface, which implies that Ni-N4/C-NH2 can immobilize CO2 •−* intermediates more strongly, finally accelerating reaction rate of CO2RR. Based on the above experimental results, the origin for enhanced catalytic activity by amination modification can be attributed to the faster charge transfer kinetics and stronger adsorption of CO2 and reaction intermediates, which was also demonstrated by DFT calculations from the perspective of catalysts electronic structure (Figure 4b-4e, and Figure S20).…”

Section: Discussionmentioning

confidence: 98%

A generalized amino-modification strategy to boost CO2 electroreduction current density of single-atom catalysts to industrial application level

Chen

Zhang

Liu

et al. 2020

Preprint

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Although Faraday efficiency (FE) for CO production of single-atom catalysts immobilized on nitrogen-doped carbon supports (M-N/C) for CO2 electrocatalytic reduction reaction (CO2RR) is generally over 90%, M-N/C catalysts demonstrate a poor reaction current density, much worse than the current density of industrial level. Herein, we first report a generalized strategy of amino-functionalized carbon supports to regulate electronic structure of M-N/C catalysts (M=Ni, Fe, Zn) to significantly increase current density of CO production. The aminated Ni single-atom catalyst achieves a remarkable CO partial current density of 447.6 mA cm-2 (a total current density over 500 mA cm-2) with a nearly 90% CO FE at a moderate overpotential of 0.89 V, and especially CO FE can be maintained over 85% in a wide operating potential range from -0.5 V to -1.0 V. DFT calculations and experimental researches demonstrate that the superior activity is attributed to enhanced adsorption energies of CO2* and COOH* intermediates caused by the change of electronic structure of aminated catalysts. This work provides an ingenious method for significantly increasing current density at industrial-relevant level of single-atom catalysts for CO2RR.

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“…The accumulation of carbon dioxide (CO 2 ) in atmosphere arising from excessive consumption of fossil fuels has triggered series of climate and environment issues . Thus effective strategies to mitigate CO 2 level and close the anthropogenic carbon cycle are critically needed.…”

Section: Figurementioning

confidence: 99%

Investigation of Structural Evolution of SnO₂ Nanosheets towards Electrocatalytic CO₂ Reduction

Liu

Dou

Wang

et al. 2020

Chemistry An Asian Journal

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In-depth understanding of the catalytic active sites is of paramount importance for the design of efficient electrocatalysts for CO 2 conversion. Here we highlight the structural evolution of SnO 2 nanosheets for electrocatalytic CO 2 reduction. The transformation of SnO 2 into metallic Sn would occur on the surface of catalyst during the catalytic process, followed by enhanced selectivity and activity for the conversion of CO 2 to HCOOH. Electrocatalytic characterization and structural analysis demonstrate that the metallic Sn derived from structural evolution plays a dominant role in the CO 2 reduction to HCOOH. This work deepens the understanding of the catalytic mechanism and provides a new pathway for the rational design of advanced electrocatalysts for CO 2 reduction.

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Simultaneous Achieving of High Faradaic Efficiency and CO Partial Current Density for CO₂ Reduction via Robust, Noble‐Metal‐Free Zn Nanosheets with Favorable Adsorption Energy

Cited by 104 publications

References 53 publications

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

A generalized amino-modification strategy to boost CO2 electroreduction current density of single-atom catalysts to industrial application level

Investigation of Structural Evolution of SnO₂ Nanosheets towards Electrocatalytic CO₂ Reduction

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Simultaneous Achieving of High Faradaic Efficiency and CO Partial Current Density for CO2 Reduction via Robust, Noble‐Metal‐Free Zn Nanosheets with Favorable Adsorption Energy

Cited by 104 publications

References 53 publications

Heterogeneous Single‐Atom Catalysts for Electrochemical CO2 Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO2 Reduction Reaction

A generalized amino-modification strategy to boost CO2 electroreduction current density of single-atom catalysts to industrial application level

Investigation of Structural Evolution of SnO2 Nanosheets towards Electrocatalytic CO2 Reduction

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Simultaneous Achieving of High Faradaic Efficiency and CO Partial Current Density for CO₂ Reduction via Robust, Noble‐Metal‐Free Zn Nanosheets with Favorable Adsorption Energy

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Heterogeneous Single‐Atom Catalysts for Electrochemical CO₂ Reduction Reaction

Investigation of Structural Evolution of SnO₂ Nanosheets towards Electrocatalytic CO₂ Reduction