Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells

Zhao, Jiwu; Huang, Liang; Xue, Lan; Niu, Zhenjie; Zhang, Zizhong; Ding, Zhengxin; Yuan, Rusheng; Lu, Xu; Long, Jinlin

doi:10.1016/j.jechem.2022.12.062

Cited by 18 publications

(3 citation statements)

References 57 publications

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“…The Raman band at 1547 cm –1 was assigned to the antisymmetrical stretching vibrations of *CO 2 . The primary detected intermediates were *HCO 3 and *COOH, with the vibration signals of 1345 cm –1 attributed to the stretching vibrations of C–O in *COOH and the Raman peak at 1425 cm –1 attributed to *HCO 3 . During the conversion process, no characteristic peaks of *CH appeared, suggesting that Zr 4+ on the material surface facilitated electronic transfer and the formation of oxygen vacancies, , which in turn promoted the transformation of intermediates from *COOH to CO.…”

Section: Resultsmentioning

confidence: 99%

“…The primary detected intermediates were *HCO 3 and *COOH, with the vibration signals of 1345 cm −1 attributed to the stretching vibrations of C−O in *COOH and the Raman peak at 1425 cm −1 attributed to *HCO 3 . 47 During the conversion process, no characteristic peaks of *CH appeared, suggesting that Zr 4+ on the material surface facilitated electronic transfer and the formation of oxygen vacancies, 48,49 which in turn promoted the transformation of intermediates from *COOH to CO. Moreover, the characteristic peaks exhibited a gradual increase in intensity with increasing temperature, indicating that higher temperatures are favorable for CO 2 conversion.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

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In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

Gao,

Yuan,

Yang

et al. 2024

ACS Sustainable Chem. Eng.

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The urgent need to address global warming has led researchers to investigate various methods for capturing and utilizing CO 2 . One promising approach is the integration of calcium looping (CaL) and reverse water−gas shift (RWGS) reactions. Therefore, dual functional materials enriched with CaZrO 3 were introduced as effective catalysts, exhibiting a sustainable catalytic CO 2 conversion to 100% CO selectivity and a remarkable CO 2 adsorption capacity (16.69 mmol g DFM −1 ), CO yield (9.64 mmol g DFM −1), even under low hydrogen concentration (15% H 2 ) in CaL and RWGS processes. Surface chemistry analysis revealed that oxygen vacancies, acting adsorption sites, and lattice oxygen of CaZrO 3 can be activated by hydrogen. This activation, linked to the formation of strong basic sites with Zr 4+ -O 2− , significantly enhanced CO 2 conversion efficiency. The synergistic promotion mechanism was validated through in situ X-ray diffraction, DRIFTS, and Raman spectroscopy techniques. The bidentate formate mechanism was predominant, indicating that bicarbonates and hydroxyl synergistic promote CO 2 conversion in the high-temperature CaL−RWGS process. 10FCZ−5 showed good long-time stability, and the material maintained a high dispersion of Fe species after 10 cycles, demonstrating excellent absorbent capacity (11 mmol g DFM −1) and CO yield (6.2 mmol g DFM −1 ).

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Section: Resultsmentioning

confidence: 99%

Section: ■ Experimental Sectionmentioning

confidence: 99%

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

Gao,

Yuan,

Yang

et al. 2024

ACS Sustainable Chem. Eng.

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“…Unlike acidic conditions, HER mechanism in an alkaline medium is hindered in the first step due to slow water dissociation. [ 16 , 17 , 18 , 19 ]…”

Section: Photoelectrochemical Water Splittingmentioning

confidence: 99%

Photoelectrocatalysis for Hydrogen Evolution Ventures into the World of Organic Synthesis

Sportelli,

Marchi,

Fornasiero

et al. 2024

Global Challenges

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The use of light as a catalytic prompt for the synthesis of industrial relevant compounds is widely explored in the past years, with a special consideration over the hydrogen evolution reaction (HER). However, semiconductors for heterogeneous photocatalysis suffer from fast charge recombination and, consequently, low solar‐to‐hydrogen efficiency. These drawbacks can be mitigated by coupling photocatalysts with an external circuit that can physically separate the photogenerated charge carriers (electrons and holes). For this reason, photoelectrochemical (PEC) production of hydrogen is under the spotlight as promising green and sustainable technique and widely investigated in numerous publications. However, considering that a significant fraction of the hydrogen produced is used for reduction processes, the development of PEC devices for direct in situ hydrogenation can address the challenges associated with hydrogen storage and distribution. This Perspective aims at highlighting the fundamental aspects of HER from PEC systems, and how these can be harnessed toward the implementation of suitable settings for the hydrogenation of organic compounds of industrial value.

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A Molecular Z‐Scheme Artificial Photosynthetic System Under the Bias‐Free Condition for CO₂ Reduction Coupled with Two‐electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H₂O₂

Kuttassery,

Ohsaki,

Thomas

et al. 2023

Angewandte Chemie

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Bio‐inspired molecular‐engineered systems have been extensively investigated for the half‐reactions of H2O oxidation or CO2 reduction with sacrificial electron donors/acceptors. However, there has yet to be reported a device for dye‐sensitized molecular photoanodes coupled with molecular photocathodes in an aqueous solution without the use of sacrificial reagents. Herein, we will report the integration of Sn(IV)‐ or Al(III)‐tetrapyridylporphyrin (SnTPyP or AlTPyP) decorated tin oxide particles (SnTPyP/SnO2 or AlTPyP/SnO2) photoanode with the dye‐sensitized molecular photocathode on nickel oxide particles containing [Ru(diimine)3]2+ as the light‐harvesting unit and [Ru(diimine)(CO)2Cl2] as the catalyst unit covalently connected and fixed within poly‐pyrrole layer (RuCAT‐RuC2‐PolyPyr‐PRu/NiO). The simultaneous irradiation of the two photoelectrodes with visible light resulted in H2O2 on the anode and mainly HCOOH with CO and H2 as minor products on the cathode with high Faradaic efficiencies in purely aqueous conditions without any applied bias is the first example of artificial photosynthesis with only two‐electron redox reactions.

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Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells

Cited by 18 publications

References 57 publications

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

Photoelectrocatalysis for Hydrogen Evolution Ventures into the World of Organic Synthesis

A Molecular Z‐Scheme Artificial Photosynthetic System Under the Bias‐Free Condition for CO₂ Reduction Coupled with Two‐electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H₂O₂

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Selectively converting CO2 to HCOOH on Cu-alloys integrated in hematite-driven artificial photosynthetic cells

Cited by 18 publications

References 57 publications

In Situ Capture and Conversion of CO2 to CO Using CaZrO3 Promoted Fe–CaO Dual-Functional Material

In Situ Capture and Conversion of CO2 to CO Using CaZrO3 Promoted Fe–CaO Dual-Functional Material

Photoelectrocatalysis for Hydrogen Evolution Ventures into the World of Organic Synthesis

A Molecular Z‐Scheme Artificial Photosynthetic System Under the Bias‐Free Condition for CO2 Reduction Coupled with Two‐electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H2O2

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In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

In Situ Capture and Conversion of CO₂ to CO Using CaZrO₃ Promoted Fe–CaO Dual-Functional Material

A Molecular Z‐Scheme Artificial Photosynthetic System Under the Bias‐Free Condition for CO₂ Reduction Coupled with Two‐electron Water Oxidation: Photocatalytic Production of CO/HCOOH and H₂O₂