Artificial photosynthetic system for diluted CO2 reduction in gas-solid phase DOI Creative Commons

Ya Wang,

Jianxin Wei, Hong‐Liang Tang

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: Oct. 11, 2024

Rational design of robust photocatalytic systems to direct capture and in-situ convert diluted CO2 from flue gas is a promising but challenging way achieve carbon neutrality. Here, we report new type host-guest photocatalysts by integrating CO2-enriching ionic liquids photoactive metal-organic frameworks PCN-250-Fe2M (M = Fe, Co, Ni, Zn, Mn) for artificial photosynthetic reduction in gas-solid phase. As result, [Emim]BF4(39.3 wt%)@PCN-250-Fe2Co exhibits record high CO2-to-CO rate 313.34 μmol g−1 h−1 under pure atmosphere 153.42 (15%) with about 100% selectivity. In scaled-up experiments 1.0 g catalyst natural sunlight irradiation, the concentration could be significantly decreased below 85% 10%, respectively, indicating its industrial application potential. Further theoretical calculations reveal that not only benefit enrichment, also form synergistic effect Co2+ sites PCN-250-Fe2Co, resulting significant Gibbs energy barrier during rate-determining step conversion. Artificial fuel authors system frameworks, greatly enhancing conversion efficiency.

Language: Английский

Metal–Organic Framework‐Based Photocatalysis for Solar Fuel Production DOI
Juan‐Ding Xiao, Rui Li, Hai‐Long Jiang

et al.

Small Methods, Journal Year: 2022, Volume and Issue: 7(1)

Published: Dec. 1, 2022

Abstract Metal–organic frameworks (MOFs) represent a novel class of crystalline inorganic–organic hybrid materials with tunable semiconducting behavior. MOFs have potential for application in photocatalysis to produce sustainable solar fuels, owing their unique structural advantages (such as clarity and modifiability) that can facilitate deeper understanding the structure–activity relationship photocatalysis. This review takes photocatalytic active sites particular perspective, summarizing progress MOF‐based fuel production; mainly including three categories solar‐chemical conversions, water splitting hydrogen fuel, carbon dioxide reduction hydrocarbon nitrogen fixation high‐energy carriers such ammonia. focuses on types photocatalysts discusses enhanced activity based well‐defined structure MOFs, offering deep insights into

Language: Английский

Citations

99
Efficient and Direct Functionalization of Allylic sp3 C−H Bonds with Concomitant CO2 Reduction DOI
Ming–Yu Qi, Yi‐Jun Xu

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(41)

Published: Aug. 26, 2023

Solar-driven CO2 reduction integrated with C-C/C-X bond-forming organic synthesis represents a substantially untapped opportunity to simultaneously tackle carbon neutrality and create an atom-/redox-economical chemical synthesis. Herein, we demonstrate the first cooperative photoredox catalysis of efficient tunable syngas, paired direct alkylation/arylation unactivated allylic sp3 C-H bonds for accessing C-C products, over SiO2 -supported single Ni atoms-decorated CdS quantum dots (QDs). Our protocol not only bypasses additional oxidant/reductant pre-functionalization substrates, affording broad products moderate excellent yields, but also produces syngas CO/H2 ratios (1 : 2-5 1). Such win-win coupling highlights high atom-, step- redox-economy, good durability, illuminating tantalizing possibility renewable sunlight-driven feedstocks manufacturing industry.

Language: Английский

Citations

80
Reversing Free‐Electron Transfer of MoS2+x Cocatalyst for Optimizing Antibonding‐Orbital Occupancy Enables High Photocatalytic H2 Evolution DOI Open Access
Duoduo Gao,

Pinsi Deng,

Jianjun Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(25)

Published: April 25, 2023

The interaction between a co-catalyst and photocatalyst usually induces spontaneous free-electron transfer them, but the effect regulation of direction on hydrogen-adsorption energy active sites have not received attention. Herein, to steer in favorable for weakening S-Hads bonds sulfur-rich MoS2+x , an electron-reversal strategy is proposed first time. core-shell Au@MoS2+x cocatalyst was constructed TiO2 optimize antibonding-orbital occupancy. Research results reveal that embedded Au can reverse electron generate electron-rich S(2+δ)- sites, thus increasing occupancy cocatalyst. Consequently, increase effectively destabilizes H 1s-p antibonding orbital weakens bond, realizing expedited desorption Hads rapidly lot visible H2 bubbles. This work delves deep into latent carrier cocatalytic activity.

Language: Английский

Citations

78
Modulating the Reaction Configuration by Breaking the Structural Symmetry of Active Sites for Efficient Photocatalytic Reduction of Low‐concentration CO2 DOI

Wenyuan Lyu,

Yang Liu,

Jingyi Zhou

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(42)

Published: Aug. 29, 2023

Photocatalytic conversion of low-concentration CO2 is considered as a promising way to simultaneously mitigate the environmental and energy issues. However, weak adsorption tough activation process seriously compromise CO production, due chemical inertness molecule formed fragile metal-C/O bond. Herein, we designed fabricated oxygen vacancy contained Co3 O4 hollow nanoparticles on ordered macroporous N-doped carbon framework (Vo-HCo3 /OMNC) towards photoreduction . In situ spectra ab initio molecular dynamics simulations reveal that constructed able break local structural symmetry Co-O-Co sites. The formation asymmetric active site switches configuration from single-site linear model multiple-sites bending one with highly stable configuration, enhancing binding polarization molecules. As result, Vo-HCo3 /OMNC shows unprecedent activity in photocatalytic (10 % /Ar) under laboratory light source or even natural sunlight, affording syngas yield 337.8 95.2 mmol g-1 h-1 , respectively, an apparent quantum up 4.2 %.

Language: Английский

Citations

76
In Situ Growth of Cs3Bi2Br9 Quantum Dots on Bi-MOF Nanosheets via Cosharing Bismuth Atoms for CO2 Capture and Photocatalytic Reduction DOI
Lan Ding, Yongping Ding,

Fenghua Bai

et al.

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(5), P. 2289 - 2303

Published: Jan. 24, 2023

Given the global warming caused by excess CO2 accumulation in atmosphere, it is essential to reduce capturing and converting chemical feedstock using solar energy. Herein, a novel Cs3Bi2Br9/bismuth-based metal-organic framework (Bi-MOF) composite was prepared via an situ growth strategy of Cs3Bi2Br9 quantum dots (QDs) on surface Bi-MOF nanosheets through coshared bismuth atoms. The Cs3Bi2Br9/Bi-MOF exhibits bifunctional merits for both high capture effective conversion CO2, among which optimized 3Cs3Bi2Br9/Bi-MOF sample shows CO2-CO yield as 572.24 μmol g-1 h-1 under irradiation 300 W Xe lamp. In addition, good stability after five recycles humid air, photoreduction efficiency does not decrease significantly. mechanistic investigation uncovers that intimate atomic-level contact between atoms only improves dispersion QDs over but also accelerates interfacial charge transfer forming strong bonding linkage, endows with best performance photoreduction. Our new finding bismuth-based framework/lead-free halide perovskite cosharing opens avenue preparation heterojunction potential applications photocatalytic CO2.

Language: Английский

Citations

68
Charging d‐Orbital Electron of ReS2+x Cocatalyst Enables Splendid Alkaline Photocatalytic H2 Evolution DOI
Wei Zhong,

Jiachao Xu,

Xidong Zhang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(36)

Published: May 14, 2023

Abstract Rhenium disulfide (ReS 2 ) holds expansive perspective in photocatalytic water‐splitting field, but its H ‐production rate is severely impeded by the strong hydroxyl (OH ad adsorption on catalytic Re atoms. Herein, an ingenious strategy about charging d ‐orbital electrons of ReS 2+x cocatalyst integrating metallic Au explicitly clarified to effectively accelerate OH desorption for promoting alkaline ‐evolution activity. To this end, core‐shell Au@ReS nanostructures as cocatalysts are skillfully fabricated onto TiO a directional assembly pathway. Experimental and theoretical data validate free‐electron transfer from core S‐rich shell, thus essentially d‐orbital atoms construct active (4‐ δ )+ sites. The charged electron state raises antibonding occupancy OH bonds, thereby accelerating endowing efficient production water splitting. Moreover, can capture photogenerated unveiled operando Kelvin probe force microscopy. Consequently, optimized /Au@ReS photocatalyst achieves exceptional 6013.45 µmol h −1 g with releasing visual bubbles media. This research furnishes original insights orbital optimize strength between intermediates

Language: Английский

Citations

63
Constructing atomic surface concaves on Bi5O7Br nanotube for efficient photocatalytic CO2 reduction DOI
Yang Wang, Kaiwen Wang,

Jiazhi Meng

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 109, P. 108305 - 108305

Published: Feb. 26, 2023

Language: Английский

Citations

49
Enhancing interfacial electric field in WO3-C3N4 through fermi level modulation for electrocatalytic nitrogen reduction DOI
Xiaoxuan Wang, Jiangzhou Xie, Shuyuan Li

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 339, P. 123126 - 123126

Published: July 22, 2023

Language: Английский

Citations

42
Dual-facet engineering of surface carboxyl functionalization and interlayer potassium ions regulation in carbon nitride for enhanced CO2 photoreduction DOI Open Access

Chen Guan,

Yulong Liao, Quanjun Xiang

et al.

Science China Materials, Journal Year: 2024, Volume and Issue: 67(2), P. 473 - 483

Published: Jan. 12, 2024

Language: Английский

Citations

41
Advances and challenges in the modification of photoelectrode materials for photoelectrocatalytic water splitting DOI

Longyue Yang,

Fang Li, Quanjun Xiang

et al.

Materials Horizons, Journal Year: 2024, Volume and Issue: 11(7), P. 1638 - 1657

Published: Jan. 1, 2024

With the increasing consumption of fossil fuels, development clean and renewable alternative fuels has become a top priority. Hydrogen (H

Language: Английский

Citations

28