Synergy of Copper Doping and Carbon Defect Engineering in Promoting C–C Coupling for Enhanced CO2 Photoreduction to Ethanol Activity DOI
Yi Zhou, Yaqi Wang, Shuo Chen

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 29, 2024

Photocatalytic conversion of carbon dioxide (CO2) to fuel provides an ideal pathway achieving neutrality. One significant hindrance in the reduction CO2 higher energy density multicarbon products (C2+) was difficulty coupling C–C bonds efficiently. Copper (Cu) is considered most suitable metal catalyst for form C2+ reaction (CO2RR), but it encounters challenges such as low product selectivity and slow catalytic efficiency. Herein, we constructed a defect on Cu-doped nitride (Cu–CvN), efficient photocatalytic CO2RR. The optimized (Cu–CvN-550) with shows high activity ethanol, ethanol production rate 122.6 μmol g–1 h–1 93.7%. yield 4.5 times than that Cu–CN-550 without defect. ratio Cu+/Cu0 Cu species changes regularly calcination temperature, which linearly correlated liquid DFT calculations combined experimental results revealed doping promoted activation, followed by enhanced *CO adsorption weakened hydrogenation desorption. Carbon defects lower free greatly accelerate transfer process promoting formation six-membered ring intermediate state, serving intramolecular dimerization. Synergistic thermodynamic kinetic interactions were realized through introduction defects, thereby enhancing performance production.

Language: Английский

Promises of MOF‐Based and MOF‐Derived Materials for Electrocatalytic CO2 Reduction DOI
Alireza Haghighat Mamaghani,

Jingwei Liu,

Zhen Zhang

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(39)

Published: July 29, 2024

Abstract Electrocatalytic CO 2 reduction (ECR) powered by renewable electricity is a promising technology to mitigate carbon emissions and lessen the dependence on fossil fuels toward carbon‐neutral energy cycle. Metal–organic frameworks (MOFs) their derivatives, due excellent intrinsic activity, have emerged as materials for ECR high‐demand products. However, challenges such unsatisfactory efficiency, selectivity, relatively low production rates hinder industrial scalability. Here, comprehensive critical review presented that summarizes state‐of‐the‐art progress in MOF‐based MOF‐derived electroreduction catalysts from design functionality perspectives. The fundamentals of reaction (CO RR) over heterogeneous catalysts, mechanisms, key faced are described first establish solid foundation forthcoming in‐depth analyses. MOF's building blocks, properties, shortcomings pertinent including conductivity stability, systematically discussed. Moreover, discussions provided design, fabrication, characterization, RR activity pinpoint intricate structure‐property‐performance relationship. Finally, recommendations put forward enhancing MOF electrocatalysts durability. This work may serve guideline developing high‐performance MOF‐related RR, benefiting researchers working this growing potentially game‐changing area.

Language: Английский

Citations

13
Recent progress in solar-driven CO2 reduction to multicarbon products DOI
Mengqian Li,

Zequn Han,

Qinyuan Hu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

Metal oxides, metal sulfides, MXenes, and metal–organic frameworks act as catalysts, while covalent organic frameworks, carbon nitrides, phosphides, graphene oxides serve cocatalysts for CO 2 photoreduction to multicarbon products.

Language: Английский

Citations

10
Research progress on photocatalysts for CO2 conversion to liquid products DOI
Linlin Wu,

Liuqing Yang,

Wenxin Liu

et al.

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: March 13, 2025

Language: Английский

Citations

1
Integration of Plasmonic Ag(I) Clusters and Fe(II) Porphyrinates into Metal‐Organic Frameworks for Efficient Photocatalytic CO2 Reduction Coupling with Photosynthesis of Pure H2O2 DOI Open Access
Huiying Chen, Jia‐Run Huang,

Jia‐Chuan Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(47)

Published: Aug. 12, 2024

Abstract Efficient photocatalytic CO 2 reduction coupled with the photosynthesis of pure H O is a challenging and significant task. Herein, using classical photoreduction site iron porphyrinate as linker, Ag(I) clusters were spatially separated evenly distributed within new metal–organic framework (MOF), namely Ag 27 TPyP‐Fe . With water electron donors, exhibited remarkable performances in artificial photosynthetic overall reaction yield 36.5 μmol g −1 h ca 100 % selectivity, well evolution rate 35.9 Since liquid phase can be more readily from gaseous products photoreduction, high‐purity concentration up to 0.1 mM was obtained. Confirmed by theoretical calculations established energy level diagram, reductive iron(II) porphyrinates oxidative an integrated functioned synergistically achieve photosynthesis. Furthermore, photoluminescence spectroscopy photoelectrochemical measurements revealed that robust connection ligands facilitated efficient charge separation rapid transfer, thereby enhancing activity.

Language: Английский

Citations

8
Recent advances of metal active sites in photocatalytic CO2 reduction DOI Creative Commons
Wa Gao, Haonan Li, Jianqiang Hu

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(35), P. 14081 - 14103

Published: Jan. 1, 2024

Photocatalytic CO

Language: Английский

Citations

7
Progress of photocatalytic CO2 reduction toward multi-carbon products DOI
Jiaojiao Fang,

Chengyang Zhu,

Hui-Ling Hu

et al.

Science China Chemistry, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 8, 2024

Language: Английский

Citations

7
Machine‐learning‐assisted intelligent synthesis of UiO‐66(Ce): Balancing the trade‐off between structural defects and thermal stability for efficient hydrogenation of Dicyclopentadiene DOI Creative Commons

Jing Lin,

Tao Ban, Li Tian

et al.

Materials Genome Engineering Advances, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 7, 2024

Abstract Metal‐organic frameworks (MOFs), renowned for structural diversity and design flexibility, exhibit potential in catalysis. However, the pursuit of higher catalytic activity through defects often compromises stability, requiring a delicate balance. Traditional trial‐and‐error method optimizing synthesis parameters within complex chemical space is inefficient. Herein, taking typical MOF UiO‐66(Ce) as an illustrative example, closed loop workflow built, which integrates machine learning (ML)‐assissted prediction, multi‐objective optimization (MOO) experimental preparation to synergistically optimize defect content thermal stability efficient hydrogenation dicyclopentadiene (DCPD). An automatic data extraction program ensures accuracy, establishing high‐quality database. ML employed explore intricate synthesis‐structure‐property correlations, enabling precise delineation pure‐phase subspace accurate predictions properties. After two iterations, MOO model identifies optimal protocols high (>40%) (>300°C). The optimized exhibits superior performance DCPD, validating precision reliability our methodology. This ML‐assisted approach offers valuable paradigm solving trade‐off riddle materials field.

Language: Английский

Citations

6
Optimizing ligand-to-metal charge transfer in metal–organic frameworks to enhance photocatalytic performance DOI
Chengzhang Zhu,

Jingkun Hou,

X.D. Wang

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 499, P. 156527 - 156527

Published: Oct. 9, 2024

Language: Английский

Citations

6
Periodic Single‐Metal Site Catalysts: Creating Homogeneous and Ordered Atomic‐Precision Structures DOI
Tianyu Zhang, Dingsheng Wang, Junfeng Liu

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(41)

Published: Aug. 16, 2024

Abstract Heterogeneous single‐metal‐site catalysts (SMSCs), often referred to as single‐atom (SACs), demonstrate promising catalytic activity, selectivity, and stability across a wide spectrum of reactions due their rationally designed microenvironments encompassing coordination geometry, binding ligands, electronic configurations. However, the inherent disorderliness SMSCs at both atomic scale nanoscale poses challenges in deciphering working principles establishing correlations between performances SMSCs. The rearrangement randomly dispersed single metals into homogeneous atomic‐precisely structured periodic single‐metal site (PSMSCs) not only simplifies chaos systems but also unveils new opportunities for manipulating performance gaining profound insights reaction mechanisms. Moreover, synergistic effects adjacent integration arrangement further broaden industrial application scope This perspective offers comprehensive overview recent advancements outlines prospective avenues research design characterizations PSMSCs, while acknowledging formidable encountered prospects that lie ahead.

Language: Английский

Citations

5
Cu-MOF composited with facet-engineered bimetallic alloys for inducing photocatalytic conversion of CO2 to C2H4 DOI
Xiangyu Lu, Peng Wang,

Zhao‐Feng Qiu

et al.

Chemical Communications, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

MIL-101(Cr) composited with Pt/Pd nanoalloy exposing the {111} facet can photocatalytically convert CO 2 to C H 4 , while one {100} has no such capability, demonstrating importance of facets in photocatalytic reduction.

Language: Английский

Citations

0