Coupling Photocatalytic Reduction and Biosynthesis Towards Sustainable CO2 Upcycling DOI Open Access
Mengjie Yu,

M. Li,

Xinzhe Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 11, 2025

Abstract Upcycling carbon dioxide (CO 2 ) into long‐chain compounds has attracted considerable attention with respect to mitigating environmental problems and obtaining value‐added feedstocks, but remains a great challenge. Herein, we report tandem photocatalysis‐biosynthesis strategy for efficient CO reduction energy‐rich sucrose or α‐farnesene. Firstly, photocatalytic of CH 4 was optimized over the transitional metal doped ZnO (M−ZnO). The as‐prepared Ni−ZnO preferentially reduces production rate 1539.1 μmol g −1 h selectivity 90 %, owing unique interface structure (Zn δ + −O−Ni β ). Subsequently, Methylomicrobium buryatense 5GB1C genetically engineered produce α‐farnesene using photocatalytically‐obtained as sole source, titer 96.3 43.9 mg L , respectively. This study provides green, low‐energy pathway synthesis from which sheds new light on tackling long‐term energy demands sustainable upcycling.

Language: Английский

Selective production of ethylene glycol at high rate via cascade catalysis DOI
Lei Fan, Yilin Zhao, Lei Chen

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(7), P. 585 - 595

Published: June 26, 2023

Language: Английский

Citations

67
Isolated Single-Atom Cobalt in the ZnIn2S4 Monolayer with Exposed Zn Sites for CO2 Photofixation DOI
Chang‐Long Tan, Ming–Yu Qi, Zi‐Rong Tang

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(12), P. 8317 - 8329

Published: June 7, 2023

Constructing highly active photocatalysts with rich reactive sites for photofixation of CO2 organic compounds implements an environmentally friendly route valorization and carbon neutralization. Herein, we report the isolated cobalt (Co) single-atom (SA)-decorated two-dimensional (2D) single-layer ZnIn2S4 (ZIS) nanosheet composites (Co-sZIS) dual centers Co Zn fixation epoxides under visible light. The unique ensemble Co-sZIS optimizes light harvesting, promotes charge carrier separation, enriches bifunctional efficient adsorption activation reactants CO2. Consequently, exhibits significantly improved CO2-epoxide cycloaddition performance compared to bulk ZIS. In addition, synergetic photoredox manner simultaneously exploiting photogenerated electrons holes efficiently facilitates epoxides, thereby further reducing energy barrier fixation. This work not only provides a paradigm rationally interfacial engineered SA-onto-2D semiconductors but also highlights structure–activity relationship by well-defined in this SA-based hybrid platform.

Language: Английский

Citations

65
Molecular tuning for electrochemical CO2 reduction DOI Creative Commons
Jincheng Zhang, Jie Ding, Yuhang Liu

et al.

Joule, Journal Year: 2023, Volume and Issue: 7(8), P. 1700 - 1744

Published: Aug. 1, 2023

Language: Английский

Citations

60
Designs of Tandem Catalysts and Cascade Catalytic Systems for CO2 Upgrading DOI

Wanzhen Zheng,

Xiaoxuan Yang, Zhongjian Li

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: June 20, 2023

Upgrading CO2 into multi-carbon (C2+) compounds through the reduction reaction (CO2 RR) offers a practical approach to mitigate atmospheric while simultaneously producing high value chemicals. The pathways for C2+ production involve multi-step proton-coupled electron transfer (PCET) and C-C coupling processes. By increasing surface coverage of adsorbed protons (*Had ) *CO intermediates, kinetics PCET can be accelerated, thereby promoting production. However, *Had are competitively intermediates on monocomponent catalysts, making it difficult break linear scaling relationship between adsorption energies /*CO intermediate. Recently, tandem catalysts consisting multicomponents have been developed improve or by enhancing water dissociation -to-CO auxiliary sites. In this context, we provide comprehensive overview design principles based products. Moreover, development cascade RR catalytic systems that integrate with downstream catalysis has expanded range potential upgrading Therefore, also discuss recent advancements in systems, highlighting challenges perspectives these systems.

Language: Английский

Citations

58
Atomically Dispersed Manganese on Carbon Substrate for Aqueous and Aprotic CO2 Electrochemical Reduction DOI
Meiling Wang, Ying Yao,

Yuhui Tian

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(12)

Published: Jan. 15, 2023

CO2 utilization and conversion are of great importance in alleviating the rising concentration atmosphere. Here, a single-atom catalyst (SAC) is reported for electrochemical both aqueous aprotic electrolytes. Specifically, atomically dispersed Mn-N4 sites embedded bowl-like mesoporous carbon particles with functionalization epoxy groups second coordination spheres. Theoretical calculations suggest that near site adjust electronic structure reduced reaction energy barriers electrocatalytic reduction to CO. The resultant Mn-single-atom N O doped (MCs-(N,O)) exhibits extraordinary performance high CO faradaic efficiency 94.5%, current density 13.7 mA cm-2 , low overpotential 0.44 V environment. Meanwhile, as cathode Li-CO2 batteries, MCs-(N,O) well-regulated active unique morphology optimizes nucleation behavior discharge products. MCs-(N,O)-based batteries deliver excellent cyclic stability 1000 h. findings this work provide new avenue design fabricate SACs various systems.

Language: Английский

Citations

47
Rationally Designed Water Enriched Nano Reactor for Stable CO2 Hydrogenation with Near 100% Ethanol Selectivity over Diatomic Palladium Active Sites DOI
Jie Chen,

Yajun Zha,

Bing Liu

et al.

ACS Catalysis, Journal Year: 2023, Volume and Issue: 13(10), P. 7110 - 7121

Published: May 10, 2023

CO2 (CO) hydrogenation presents the widest route to synthesis of various valuable organic molecules, but precise carbon–carbon coupling control targeted products along with elimination byproducts remains a challenge. We overcome these limitations by synthesizing CeO2-supported dual Pd site catalyst that could actively catalyze conversion into single-product ethanol almost without C1 in continuous-flow fixed-bed reactor. This surprising finding is derived from observation synergistic catalysis between atoms leads extraordinary ability for cleavage C–O bond *CHxOH species and *CHx *CO species. Furthermore, sites be stabilized through enriching situ formed water nano reactor hydrophobic shell layer, thus leading remarkably improved catalytic stability production. As result, as-constructed exhibited superior selectivity at 98.7%, corresponding productivity up 11.6 g per gram hour excellent during continuous test 60 h. Our results demonstrate multifunctional active can break restriction reaction involving single catalyst.

Language: Английский

Citations

47
Selective synthesis of butane from carbon monoxide using cascade electrolysis and thermocatalysis at ambient conditions DOI
Mi Gyoung Lee‬, Xiaoyan Li, Adnan Ozden

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(4), P. 310 - 318

Published: April 3, 2023

Language: Английский

Citations

46
Bioelectrocatalysis for CO2 reduction: recent advances and challenges to develop a sustainable system for CO2 utilization DOI

Likun Luan,

Xiuling Ji,

Boxia Guo

et al.

Biotechnology Advances, Journal Year: 2023, Volume and Issue: 63, P. 108098 - 108098

Published: Jan. 14, 2023

Language: Английский

Citations

45
Engineering extracellular electron transfer pathways of electroactive microorganisms by synthetic biology for energy and chemicals production DOI
Junqi Zhang, Feng Li,

Dingyuan Liu

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 53(3), P. 1375 - 1446

Published: Dec. 20, 2023

The excessive consumption of fossil fuels causes massive emission CO

Language: Английский

Citations

43
Nanocellulose‐Assisted Molecularly Engineering of Nitrogen Deficient Graphitic Carbon Nitride for Selective Biomass Photo‐Oxidation DOI

Ren Zou,

Zhongxin Chen, Linxin Zhong

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(29)

Published: May 1, 2023

Abstract Structural modulation of graphitic carbon nitride (g‐C 3 N 4 ) remains a major challenge in rational catalyst design for artificial photosynthesis valuable chemicals. Herein, cellulose nanofiber (CNF) assisted polymerization is utilized to prepare 1D holey g‐C nanorods (HCN) with nitrogen vacancies and oxygen dopants photochemical synthesis lactic acid via monosaccharide photooxidation. The HCN exhibits remarkable yield 75.5% from wide assortment sugars such as hexose (C5) pentose (C6), together an excellent hydrogen production rate 2.8 mmol h −1 g . Mechanistic studies confirm the rapid generation superoxide radical responsible superior activity, enjoying synergetic effect between dopants. This work provides new directions green efficient photocatalysts biomass upgrading.

Language: Английский

Citations

42