Fabrication of Flexible Mesoporous Black Nb2O5 Nanofiber Films for Visible‐Light‐Driven Photocatalytic CO2 Reduction into CH4 DOI
Xi Lin,

Shuhui Xia,

Liang Zhang

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(16)

Published: Feb. 19, 2022

Achieving high selectivity and conversion efficiency simultaneously is a challenge for visible-light-driven photocatalytic CO2 reduction into CH4 . Here, facile nanofiber synthesis method new defect control strategy at room-temperature are reported the fabrication of flexible mesoporous black Nb2 O5 catalysts that contain abundant oxygen-vacancies unsaturated Nb dual-sites, which efficient towards production The oxygen-vacancy decreases bandgap width from 3.01-2.25 eV, broadens light-absorption range ultraviolet to visible-light, dual sites in mesopores can easily adsorb , so intermediate product CO* be spontaneously changed *CHO. formation highly stable NbCHO* proposed key feature determining selectivity. preliminary results show without using sacrificial agents photosensitizers, catalyst achieves 64.8% with evolution rate 19.5 µmol g-1 h-1 under visible-light. Furthermore, film directly used devices, showing appealing broadly commercial applications.

Language: Английский

Doping regulation in transition metal compounds for electrocatalysis DOI
An Zhang, Yongxiang Liang, Han Zhang

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(17), P. 9817 - 9844

Published: Jan. 1, 2021

This review summarizes the recent progress related to field of doping regulation in transition metal compounds, aiming give an overview this strategy for designing high-performance catalysts towards electrocatalytic applications.

Language: Английский

Citations

428
Photocatalytic CO2 reduction DOI
Siyuan Fang, Motiar Rahaman, Jaya Bharti

et al.

Nature Reviews Methods Primers, Journal Year: 2023, Volume and Issue: 3(1)

Published: Aug. 10, 2023

Language: Английский

Citations

330
Modulating electron density of vacancy site by single Au atom for effective CO2 photoreduction DOI Creative Commons
Yuehan Cao,

Lan Guo,

Meng Dan

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: March 15, 2021

Abstract The surface electron density significantly affects the photocatalytic efficiency, especially CO 2 reduction reaction, which involves multi-electron participation in conversion process. Herein, we propose a conceptually different mechanism for modulation based on model of Au anchored CdS. We firstly manipulate direction transfer by regulating vacancy types When electrons accumulate vacancies instead single atoms, adsorption change from physical to chemical adsorption. More importantly, is manipulated controlling size nanostructures. nanoclusters downsize strong hybridization 5 d and S p orbits accelerates photo-electrons onto surface, resulting more available reduction. As result, product generation rate SA /Cd 1−x manifests remarkable at least 113-fold enhancement compared with pristine Cd S.

Language: Английский

Citations

299
Architectural Design for Enhanced C2 Product Selectivity in Electrochemical CO2 Reduction Using Cu-Based Catalysts: A Review DOI
Changlong Xiao, Jie Zhang

ACS Nano, Journal Year: 2021, Volume and Issue: 15(5), P. 7975 - 8000

Published: May 6, 2021

Electrochemical CO2 reduction to value-added chemicals and fuels is a promising approach mitigate the greenhouse effect arising from anthropogenic emission energy shortage caused by depletion of nonrenewable fossil fuels. The generation multicarbon (C2+) products, especially hydrocarbons oxygenates, great interest for industrial applications. To date, Cu only metal known catalyze C–C coupling in electrochemical reaction (eCO2RR) with appreciable efficiency kinetic viability produce wide range C2 products aqueous solutions. Nonetheless, poor product selectivity associated main technical problem application eCO2RR technology on global scale. Based extensive research efforts, delicate rational design electrocatalyst architecture using principles nanotechnology likely significantly affect adsorption energetics some key intermediates hence inherent pathways. In this review, we summarize recent progress that has been achieved tailoring efficient conversion target products. By considering experimental computational results, further analyze underlying correlations between catalyst its toward Finally, major challenges are outlined, directions future development suggested.

Language: Английский

Citations

267
Metal–Organic Frameworks as Photocatalysts for Solar-Driven Overall Water Splitting DOI Creative Commons
Sergio Navalón, Amarajothi Dhakshinamoorthy, Mercedes Álvaro

et al.

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(1), P. 445 - 490

Published: Dec. 12, 2022

Metal–organic frameworks (MOFs) have been frequently used as photocatalysts for the hydrogen evolution reaction (HER) using sacrificial agents with UV–vis or visible light irradiation. The aim of present review is to summarize use MOFs solar-driven targeting overcome current efficiency limitations in overall water splitting (OWS). Initially, fundamentals photocatalytic OWS under solar irradiation are presented. Then, different strategies that can be implemented on adapt them photocatalysis discussed detail. Later, most active reported until now HER and/or oxygen (OER) critically commented. These studies taken precedents discussion existing sunlight requirements met at large scale also discussed. last section this provides a summary state field and comments future prospects could bring closer commercial application.

Language: Английский

Citations

257
Engineering a local acid-like environment in alkaline medium for efficient hydrogen evolution reaction DOI Creative Commons
Hao Tan,

Bing Tang,

Ying Lü

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: April 19, 2022

Tuning the local reaction environment is an important and challenging issue for determining electrochemical performances. Herein, we propose a strategy of intentionally engineering to yield highly active catalysts. Taking Ptδ- nanoparticles supported on oxygen vacancy enriched MgO nanosheets as prototypical example, have successfully created acid-like in alkaline medium achieve excellent hydrogen evolution The evidenced by operando Raman, synchrotron radiation infrared X-ray absorption spectroscopy that observes key H3O+ intermediate emergence surface accumulation around sites during electrocatalysis. Further analysis confirms critical factors forming include: facilitates H2O dissociation generate species; F centers transfers its unpaired electrons Pt, leading formation electron-enriched positively charged migrates negatively accumulates due electrostatic attraction, thus creating acidic medium.

Language: Английский

Citations

236
Construction of C–N bonds from small-molecule precursors through heterogeneous electrocatalysis DOI
Junnan Li, Yuxuan Zhang,

Kiran Kuruvinashetti

et al.

Nature Reviews Chemistry, Journal Year: 2022, Volume and Issue: 6(5), P. 303 - 319

Published: April 25, 2022

Language: Английский

Citations

233
Selective photocatalytic CO2 reduction in aerobic environment by microporous Pd-porphyrin-based polymers coated hollow TiO2 DOI Creative Commons
Yajuan Ma,

Xiaoxuan Yi,

Shaolei Wang

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: March 17, 2022

Abstract Direct photocatalytic CO 2 reduction from primary sources, such as flue gas and air, into fuels, is highly desired, but the thermodynamically favored O almost completely impedes this process. Herein, we report on efficacy of a composite photocatalyst prepared by hyper-crosslinking porphyrin-based polymers hollow TiO surface subsequent coordinating with Pd(II). Such exhibits high resistance against inhibition, leading to 12% conversion yield air after 2-h UV-visible light irradiation. In contrast, over Pd/TiO without polymer severely inhibited presence ( ≥ 0.2 %). This study presents feasible strategy, building Pd(II) sites -adsorptive surface, for realizing H in an aerobic environment /O adsorption selectivity efficient charge separation oxidation , respectively.

Language: Английский

Citations

225
Role of oxygen vacancy in metal oxides for photocatalytic CO2 reduction DOI
Wenbin Jiang,

Hongyi Loh,

Beverly Qian Ling Low

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 122079 - 122079

Published: Oct. 17, 2022

Language: Английский

Citations

219
Sub‐Second Time‐Resolved Surface‐Enhanced Raman Spectroscopy Reveals Dynamic CO Intermediates during Electrochemical CO2 Reduction on Copper DOI Creative Commons
Hongyu An, Longfei Wu, Laurens D. B. Mandemaker

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(30), P. 16576 - 16584

Published: April 15, 2021

Abstract The electrocatalytic carbon dioxide (CO 2 ) reduction reaction RR) into hydrocarbons is a promising approach for greenhouse gas mitigation, but many details of this dynamic remain elusive. Here, time‐resolved surface‐enhanced Raman spectroscopy (TR‐SERS) employed to successfully monitor the dynamics CO RR intermediates and Cu surfaces with sub‐second time resolution. Anodic treatment at 1.55 V vs. RHE subsequent surface oxide (below −0.4 RHE) induced roughening electrode surface, which resulted in hotspots TR‐SERS, enhanced resolution (down ≈0.7 s) fourfold improved efficiency toward ethylene. With initial restructuring was followed (<7 s), after stable surrounded by increased local alkalinity formed. Our measurements revealed that highly intermediate, characteristic vibration below 2060 cm −1 , related C−C coupling ethylene production (−0.9 RHE), whereas lower cathodic bias (−0.7 gaseous from isolated static species distinct 2092 .

Language: Английский

Citations

217