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

Solar‐Driven Conversion of CO2 to C2 Products by the 3d Transition Metal Intercalates of Layered Lead Iodides DOI

Jinlin Yin,

Dongyang Li, Chen Sun

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(30)

Published: May 2, 2024

Abstract Photocatalytic CO 2 reduction to high‐value‐added C 2+ products presents significant challenges, which is attributed the slow kinetics of multi‐e − photoreduction and high thermodynamic barrier for C–C coupling. Incorporating redox‐active Co /Ni cations into lead halide photocatalysts has potentials improve carrier transport introduce charge polarized bimetallic sites, addressing kinetic issues, respectively. In this study, a coordination‐driven synthetic strategy developed 3d transition metals interlamellar region layered organolead iodides with atomic precision. The resultant hybrids exhibit selective H 5 OH using O vapor at evolution rates 24.9–31.4 µmol g −1 h selectivity 89.5–93.6%, while pristine iodide yields only 1 products. Band structure calculations photoluminescence studies indicate that interlayer species greatly contribute frontier orbitals enhance exciton dissociation free carriers, facilitating between adjacent layers. addition, Bader distribution in situ experimental spectroscopic reveal asymmetric Ni–O–Pb catalytic sites intrinsic polarization, promoting coupling leading formation key *OC–CHO intermediate.

Language: Английский

Citations

15
Regulating COOH Intermediate via Rationally Constructed Surface‐Active Sites of Bi2WO6 for Solar‐Driven CO2‐to‐CO Production DOI Open Access
Nguyen Quoc Thang, Amr Sabbah, P. Raghunath

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 7, 2025

Abstract Solar‐driven CO 2 reduction holds great promise for sustainable energy, yet the role of atomic active sites in governing intermediate formation and conversion remains poorly understood. Herein, a synergistic strategy using Ni single atoms (SAs) surface oxygen vacancies (O v ) is reported to regulate pathway on Bi WO 6 photocatalyst. Combining in‐situ techniques theoretical modeling, reaction mechanism structure‐activity relationship elucidated. In‐situ X‐ray absorption spectroscopy identifies as sites, diffuse reflectance infrared Fourier transform demonstrates that adsorption H O readily forms 3 2− species ‐rich catalyst. Optimally balancing SAs lowers energy barrier dehydration key COOH intermediate, leading favorable desorption. Consequently, superior production efficiency 53.49 µmol g ‒1 achieved, surpassing previous reports ‐based catalysts gas‐phase photoreduction.

Language: Английский

Citations

1
Enhanced g-C3N4 photocatalytic removal of tetracycline under visible light: Synergistic effect of N vacancies and Ni, Zr co-doping DOI
Peng Wang, Hai‐Tao Ren, Xinxin Yu

et al.

Journal of Photochemistry and Photobiology A Chemistry, Journal Year: 2025, Volume and Issue: unknown, P. 116308 - 116308

Published: Jan. 1, 2025

Language: Английский

Citations

1
Polarized microenvironment-modulated covalent organic frameworks with nickel single atoms for enhanced CO2 photoreduction DOI

Piyan Wang,

Ying Dai, Zhenyu Song

et al.

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 162084 - 162084

Published: March 1, 2025

Language: Английский

Citations

1
Covalent triazine frameworks materials for photo- and electro-catalysis DOI

Aoji Liang,

Wenbin Li,

Anbai Li

et al.

Nano Research, Journal Year: 2024, Volume and Issue: 17(9), P. 7830 - 7839

Published: June 29, 2024

Language: Английский

Citations

8
Porous Organic Polymers with Shiftable Active Co(II) Sites for Photocatalytic Reduction of CO2 to C2H4 DOI
Keke Wang, Qiang Li,

Xiahe Chen

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 362, P. 124765 - 124765

Published: Oct. 30, 2024

Language: Английский

Citations

6
Targeting active sites nickel-porphyrin over BiOBr nanosheets with excellent charge separation for accelerated photoreduction reactions DOI
Lina Li, Gaopeng Liu,

Shengqun Cao

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: unknown, P. 124904 - 124904

Published: Dec. 1, 2024

Language: Английский

Citations

5
Plasma–Liquid‐Induced Synthesis of Scandium–Metalloporphyrin Frameworks for Boosted Sensing and Photosensitization DOI Open Access

Zhankuo Zhang,

Zhaohui Liu,

Xueshan Chen

et al.

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 5, 2025

Inserting metal ions into the porphyrin ring is one of primary strategies to enhance properties porphyrin-based metal-organic frameworks (MOFs). However, straightforward, rapid, and energy-efficient synthesis MOFs with high metallization for remains challenging. Herein, a solution anode glow discharge (SAGD) microplasma presented one-step scandium-metalloporphyrin (ScMPFs). The substantial number electrons provided by plasma-liquid interface not only accelerated rapid nucleation growth but also promoted incorporation scandium (Sc

Language: Английский

Citations

0
Breaking the structural symmetry of active sites in zeolite imidazolate framework for enhanced CO2 photoreduction DOI

Yu-Peng Han,

Yayu Yan,

Qiaohong Li

et al.

Science China Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 3, 2025

Language: Английский

Citations

0
Biomimetic Construction of Ferriporphyrin‐Based Porous Catalysts for Boosting Nitrogen Electroxidation to Nitrate DOI Open Access
Hongming He, Shan Zhang, Yongling An

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 19, 2025

Abstract Electrocatalytic N 2 oxidation reaction (NOR) is an environmentally sustainable approach to synthesize NO 3 − under mild conditions. Inspired by the ferriporphyrin (FePP) catalytic species in nitrite oxidoreductase, three FePP‐based biomimetic catalysts with different functional groups (─NH , ─H, and ─COOCH ) are designed prepared successfully. Theoretical calculations indicate that these can alter electron density of Fe center, affecting their ability adsorb activate . The strong electron‐donating ─NH group enhance iron sites, which reveals a maximum yield 728.55 µmol h −1 g FePP high Faradaic efficiency 10.6%. After that, optimized molecules be encapsulated into ZIF‐8, remarkably promoted ─to─NO transformation production rate 1767.74 achieving highest effect among metalloporphyrin‐based molecular This work develops available modulate distribution active metal sites confine porous crystalline materials for constructing high‐performance NOR electrocatalysts.

Language: Английский

Citations

0