Efficient hybrid solar-to-alcohol system via synergistic catalysis between well-defined Cu–N4 sites and its sulfide (CuS)

Cheng, Jun; Yang, Xiao Qing; Xuan, Xiaoxu; Zhou, Junhu

doi:10.1016/j.cej.2019.123799

Cited by 8 publications

(9 citation statements)

References 31 publications

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“…This value is significantly higher than that of NC (0.41 mmol·g –1 ). The large CO 2 adsorption capability of the catalyst enables the adsorption of a large amount of CO 2 onto the NiPc/NC surface, resulting in a significant increase in its catalytic performance. − …”

Section: Resultsmentioning

confidence: 99%

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Yang

Cheng

Xuan

et al. 2020

ACS Sustainable Chem. Eng.

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To enhance the faradic efficiency of the electrocatalytic CO2 reduction reaction (CO2RR) with stable catalysts, atomically dispersed Ni–N5 active sites composed of planar Ni–N4 (in nickel phthalocyanine) coordinated with the N atom in the carbon matrix (denoted as NiPc/NC) were proposed to reduce CO2 into CO products. Extended X-ray absorption fine structure (EXAFS) spectroscopy and aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) measurements confirmed that the Ni–N5 structure composed of single Ni atoms in NiPc and N doped in the carbon matrix. Density functional theory (DFT) calculations reveal that an energy barrier of only +0.89 eV is required for the process to take place on the surface of NiPc@pyridinic N. This barrier is significantly lower than in the case of NiPc@graphitic N (+2.12 eV), NiPc@pyrrolic N (+1.60 eV), and NiPc@C (+2.64 eV). This result suggests that the high CO2RR activity originates from the synergistic effect between the coordinatively unsaturated Ni–N4 sites and the surface pyridinic N species. The faradic efficiency of CO2 reduction into the CO product was ≥93% over the NiPc/NC catalyst in a wide potential range of −0.5 to −0.8 V (vs a reversible hydrogen electrode, RHE). The peak CO faradic efficiency was 98% at a potential of −0.5 V due to the synergistic effect of Ni–N4 sites in NiPc and pyridinic N atom doped in NC.

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Section: Resultsmentioning

confidence: 99%

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Yang

Cheng

Xuan

et al. 2020

ACS Sustainable Chem. Eng.

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“…Another report by Cheng and co-workers used the Cu( ii )- meso -tetra- p -carboxyphenyl-porphyrin to prepare PMOFs nanosheets (NSs) on top of which CuS NPs were attached providing the catalytic moieties for CO 2 reduction. 291 This catalytic system was employed as electrocathode for CO 2 conversion in the two-compartments photoelectrochemical cell with TiO 2 nanotube photoanodes performing water oxidation (Fig. 61d) and exhibited efficient and selective light induced CO 2 conversion to ethanol (Table 13, entry 11).…”

Section: Porphyrins For Co2 Reductionmentioning

confidence: 99%

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

et al. 2022

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“…It comprises uniformly distributed Cu ions as active centers for an enhanced catalytic performance . The microstructure characteristics of the hybrid composite of CuS/CuPor-based MOF nanosheets were assessed by SEM and HR-TEM studies . The SEM analysis, along with fractal dimensional studies, revealed that performing the sulfuration for 4 h resulted in an increase in fractal dimension, which was ascribed to CuS NPs formation on the CuPor nanosheets, resulting in a greater number of pores and corrugations.…”

Section: Mofs As a Host Materials For Anchoring Sacs And Nmtsmentioning

confidence: 99%

Emerging Single-Atom Catalysts and Nanomaterials for Photoelectrochemical Reduction of Carbon Dioxide to Value-Added Products: A Review of the Current State-of-the-Art and Future Perspectives

Verma

Yadav

2023

Energy Fuels

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Rapid industrialization has resulted in a drastic increase in the consumption of natural resources, particularly fossil fuels. Fossil fuels in the form of coal, natural gas, oils, etc. have been extensively used to meet ever-increasing energy demands, resulting in adverse environmental effects. Massive fossil fuel consumption has led to enormous carbon dioxide (CO2) emissions, adversely impacting the environment through global warming. Photoelectrochemical (PEC) reduction of CO2 into valuable fuels, for instance, formic acid (HCOOH), methanol (CH3OH), ethanol (C2H5OH), etc., which combines the merits of both photochemical and electrochemical techniques, has been considered as a potential approach to address the issue of CO2 mitigation. Single-atom catalysts (SACs) along with emerging nanomaterials (NMTs) as photoelectrode composite materials present an effective avenue to augment PEC CO2 reduction owing to their well-defined structures and almost complete atom utilization. The present review focuses on the application of various SACs and NMTs as emerging photoelectrode materials that are advantageous for efficient PEC CO2 reduction to valuable fuels, such as HCOOH, CH3OH, C2H5OH, and carbon monoxide. The mechanism pertaining to the effective utilization of incident light energy to overcome the band gap and produce photogenerated charge carriers that contribute to the PEC reduction of CO2 has also been elucidated. At the outset, some challenges and opportunities that lie ahead in boosting SAC’s PEC performance have been discussed.

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Efficient hybrid solar-to-alcohol system via synergistic catalysis between well-defined Cu–N4 sites and its sulfide (CuS)

Cited by 8 publications

References 31 publications

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction

Emerging Single-Atom Catalysts and Nanomaterials for Photoelectrochemical Reduction of Carbon Dioxide to Value-Added Products: A Review of the Current State-of-the-Art and Future Perspectives

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Efficient hybrid solar-to-alcohol system via synergistic catalysis between well-defined Cu–N4 sites and its sulfide (CuS)

Cited by 8 publications

References 31 publications

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N4 Sites for Electrocatalytic CO2 Reduction

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N4 Sites for Electrocatalytic CO2 Reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H2production and CO2reduction

Emerging Single-Atom Catalysts and Nanomaterials for Photoelectrochemical Reduction of Carbon Dioxide to Value-Added Products: A Review of the Current State-of-the-Art and Future Perspectives

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Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Boosting Defective Carbon by Anchoring Well-Defined Atomically Dispersed Ni–N₄ Sites for Electrocatalytic CO₂ Reduction

Porphyrins and phthalocyanines as biomimetic tools for photocatalytic H₂production and CO₂reduction