Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO2Conversion DOI
Honghui Ou, Shangbo Ning, Peng Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(34)

Published: June 18, 2022

Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO2 conversion. However, designing active sites for reduction and H2 O oxidation simultaneously on a photocatalyst combining corresponding half-reaction system is still difficult. Here, we synthesized bimetallic single-atom with two compatible centers Mn Co carbon nitride (Mn1 Co1 /CN). Our experimental results density functional theory calculations showed that center promotes by accumulating photogenerated holes. In addition, activation increasing bond length angle molecules. Benefiting from synergistic effect atomic centers, Mn1 /CN exhibited CO production rate 47 μmol g-1 h-1 , which significantly higher than single-metal photocatalyst.

Language: Английский

A review on heterogeneous photocatalysis for environmental remediation: From semiconductors to modification strategies DOI
Huijie Wang, Xin Li, Xiaoxue Zhao

et al.

CHINESE JOURNAL OF CATALYSIS (CHINESE VERSION), Journal Year: 2022, Volume and Issue: 43(2), P. 178 - 214

Published: Jan. 17, 2022

Language: Английский

Citations

625

A Review of MOFs and Their Composites‐Based Photocatalysts: Synthesis and Applications DOI
Yongteng Qian, Fangfang Zhang, Huan Pang

et al.

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(37)

Published: June 26, 2021

Abstract Photocatalysis is considered to be a green and environment‐friendly technology since it can convert solar energy into other types of chemical energies. Over the past several years, metal‐organic frameworks (MOFs)‐based photocatalysts have received remarkable research interest due their unique morphology, high photocatalytic performance, good stability, easy synthesis, low cost. In this review, synthetic strategies developing MOFs‐based are first introduced. Second, recent progress in fabrication various MOFs composites summarized. Third, different applications including hydrogen evolution reaction, oxygen overall water splitting, nitrogen reduction carbon dioxide reaction as well photodegradation organic pollutants summed up. Finally, challenges some suggestions for future development MOFs‐ composites‐based also highlighted. It expected that report will help researchers systematically devise develop highly efficient based on composites.

Language: Английский

Citations

385

Single-atom catalysts for photocatalytic energy conversion DOI Creative Commons
Zhonghua Xue, Deyan Luan, Huabin Zhang

et al.

Joule, Journal Year: 2022, Volume and Issue: 6(1), P. 92 - 133

Published: Jan. 1, 2022

Artificial photocatalytic energy conversion represents a highly intriguing strategy for solving the crisis and environmental problems by directly harvesting solar energy. The development of efficient photocatalysts is central task pushing real-world application reactions. Due to maximum atomic utilization efficiency distinct advantages outstanding catalytic activity, single-atom catalysts (SACs) have emerged as promising candidates photocatalysts. In current review, recent progresses challenges on SACs systems are presented. Fundamental principles focusing charge separation/transfer molecular adsorption/activation photocatalysis systemically explored. We outline how isolated reactive sites facilitate photogenerated electron–hole transfer promote construction photoactivation cycles. widespread adoption in diverse reactions also comprehensively introduced. By presenting these advances addressing some future with potential solutions related integral over SACs, we expect shed light forthcoming research conversion.

Language: Английский

Citations

380

Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis DOI Creative Commons
Hongyu Jing, Peng Zhu, Xiaobo Zheng

et al.

Advanced Powder Materials, Journal Year: 2021, Volume and Issue: 1(1), P. 100013 - 100013

Published: Nov. 15, 2021

Various metal-based electrocatalysts from nanocrystals, to clusters and single-atoms, have been well-discovered towards high-efficient power devices electrocatalytic conversion. To accelerate energy transformation materials discovery, developing high-throughput DFT calculations machine-learning techniques is of great necessity. This review comprehensively outlines the latest progress theory-guided design advanced materials. Especially, we focus on study single atoms in various devices, such as fuel cell (oxygen reduction reaction, ORR; acid oxidation reaction; alcohol reaction), other reactions for energy-related conversion small molecules, H2O2 evolution (2e− ORR), water splitting (H2 reaction/O2 HER/OER), N2 reaction (NRR), CO2 (CO2RR). Firstly, electronic structure, interaction mechanism, activation path are discussed provide an overall blueprint electrocatalysis batteries mentioned above. Thereafter, experimental synthesis strategies, structural recognition, performance figured out. Finally, some viewpoints into current issues future concept provided.

Language: Английский

Citations

376

Photocatalytic C–C Coupling from Carbon Dioxide Reduction on Copper Oxide with Mixed-Valence Copper(I)/Copper(II) DOI
Wei Wang, Chaoyuan Deng,

Shijie Xie

et al.

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(7), P. 2984 - 2993

Published: Feb. 11, 2021

To realize the evolution of C2+ hydrocarbons like C2H4 from CO2 reduction in photocatalytic systems remains a great challenge, owing to gap between relatively lower efficiency multielectron transfer photocatalysis and sluggish kinetics C–C coupling. Herein, with Cu-doped zeolitic imidazolate framework-8 (ZIF-8) as precursor, hybrid photocatalyst (CuOX@p-ZnO) CuOX uniformly dispersed among polycrystalline ZnO was synthesized. Upon illumination, catalyst exhibited ability reduce 32.9% selectivity, rate 2.7 μmol·g–1·h–1 water hole scavenger high 22.3 presence triethylamine sacrificial agent, all which have rarely been achieved systems. The X-ray absorption fine structure spectra coupled situ FT-IR studies reveal that, original catalyst, Cu mainly existed form CuO, while unique Cu+ surface layer upon CuO matrix formed during reaction, this site is active anchor generated CO further perform coupling C2H4. intermediate *OC–COH experimentally identified by for first time reduction. Moreover, theoretical calculations showed critical role such sites strengthening binding *CO stabilizing intermediate. This work uncovers new paradigm achieve system.

Language: Английский

Citations

343

Single-atom Cu anchored catalysts for photocatalytic renewable H2 production with a quantum efficiency of 56% DOI Creative Commons
Yumin Zhang, Jianhong Zhao, Hui Wang

et al.

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

Published: Jan. 10, 2022

Abstract Single-atom catalysts anchoring offers a desirable pathway for efficiency maximization and cost-saving photocatalytic hydrogen evolution. However, the single-atoms loading amount is always within 0.5% in most of reported due to agglomeration at higher concentrations. In this work, highly dispersed large (>1 wt%) copper were achieved on TiO 2 , exhibiting H evolution rate 101.7 mmol g −1 h under simulated solar light irradiation, which than other photocatalysts reported, addition excellent stability as proved after storing 380 days. More importantly, it exhibits an apparent quantum 56% 365 nm, significant breakthrough field. The Cu incorporation enables efficient electron transfer via 2+ -Cu + process. present approach paves way design advanced materials remarkable activity durability.

Language: Английский

Citations

343

Advances in the Development of Single‐Atom Catalysts for High‐Energy‐Density Lithium–Sulfur Batteries DOI
Ziwei Liang, Jiadong Shen, Xijun Xu

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(30)

Published: March 3, 2022

Abstract Although lithium–sulfur (Li–S) batteries are promising next‐generation energy‐storage systems, their practical applications limited by the growth of Li dendrites and lithium polysulfide shuttling. These problems can be mitigated through use single‐atom catalysts (SACs), which exhibit advantages maximal atom utilization efficiency (≈100%) unique catalytic properties, thus effectively enhancing performance electrode materials in devices. This review systematically summarizes recent progress SACs intended for Li‐metal anodes, S cathodes, separators, briefly introducing operating principles Li–S batteries, action mechanisms corresponding SACs, fundamentals activity, then comprehensively describes main strategies synthesis. Subsequently, operation reinforced as well other metal–S individually illustrated, major challenges usage future development directions presented.

Language: Английский

Citations

336

Engineering Single-Atom Active Sites on Covalent Organic Frameworks for Boosting CO2 Photoreduction DOI
Lei Ran,

Zhuwei Li,

Bei Ran

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(37), P. 17097 - 17109

Published: Sept. 6, 2022

Solar carbon dioxide (CO2) conversion is an emerging solution to meet the challenges of sustainable energy systems and environmental/climate concerns. However, construction isolated active sites not only influences catalytic activity but also limits understanding structure-catalyst relationship CO2 reduction. Herein, we develop a universal synthetic protocol fabricate different single-atom metal (e.g., Fe, Co, Ni, Zn, Cu, Mn, Ru) anchored on triazine-based covalent organic framework (SAS/Tr-COF) backbone with bridging structure metal-nitrogen-chlorine for high-performance Remarkably, as-synthesized Fe SAS/Tr-COF as representative catalyst achieved impressive CO generation rate high 980.3 μmol g-1 h-1 selectivity 96.4%, over approximately 26 times higher than that pristine Tr-COF under visible light irradiation. From X-ray absorption fine analysis density functional theory calculations, superior photocatalytic performance attributed synergic effect atomically dispersed host, decreasing reaction barriers formation *COOH intermediates promoting adsorption activation well desorption. This work affords rational design state-of-the-art catalysts at molecular level provides in-depth insights efficient conversion.

Language: Английский

Citations

330

Green Carbon Science: Efficient Carbon Resource Processing, Utilization, and Recycling towards Carbon Neutrality DOI
Mingyuan He, Yuhan Sun, Buxing Han

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 61(15)

Published: Dec. 17, 2021

Green carbon science is defined as the "study and optimization of transformation carbon-containing compounds relevant processes involved in entire cycle from resource processing, energy utilization, CO2 fixation, recycling to utilize resources efficiently minimize net emission."[1] related closely neutrality, fields have developed quickly last decade. In this Minireview, we propose concept index, recent progress petroleum refining, production liquid fuels, chemicals, materials using coal, methane, , biomass, waste plastics highlighted combination with green science. An outlook for these important provided final section.

Language: Английский

Citations

315

Dual optimization approach to Mo single atom dispersed g-C3N4 photocatalyst: Morphology and defect evolution DOI
Chen Zhang, Deyu Qin, Yin Zhou

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 303, P. 120904 - 120904

Published: Nov. 7, 2021

Language: Английский

Citations

313