Facilitating Molecular Activation and Proton Feeding by Dual Active Sites on Polymeric Carbon Nitride for Efficient CO2Photoreduction DOI

Xiaoqiang An,

Qingwen Tang,

Huachun Lan

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(46)

Published: Sept. 23, 2022

Photoreduction of CO2 provides an appealing way to alleviate the energy crisis and manage global carbon balance but is limited by high activation rate-limiting proton transfer. We now develop a dual-site strategy for high-efficiency conversion through polarizing molecules at pyridine N vacancies accelerating intermediate protonation protonated adjacent nitrogen on polymeric nitride. Our photocatalysts with atomic-level engineered active sites manifest CO production rate 1835 μmol g-1 h-1 , 183 times higher than pristine bulk Theoretical prediction experimental studies confirm that such excellent performance attributed synergistic effect between vacant in decreasing formation key *COOH intermediates efficient electron transfer relay facilitated defect-induced shallow trap state homogeneous charge mediators.

Language: Английский

Atomically Dispersed Metal‐Based Catalysts for Zn–CO2Batteries DOI Creative Commons

Sanshuang Gao,

Tianran Wei, Jiaqiang Sun

et al.

Small Structures, Journal Year: 2022, Volume and Issue: 3(12)

Published: Aug. 19, 2022

Rechargeable aqueous Zn–CO 2 batteries show great promise in meeting severe environmental problems and energy crises due to their combination of CO utilization output, as well advantages high theoretical density, abundant raw materials, safety. Developing high‐efficiency stable reduction reaction (CO RR) electrocatalysts is critical importance for the promotion this technology. Atomically dispersed metal‐based catalysts (ADMCs), with extremely atom‐utilization efficiency, tunable coordination environments, superior intrinsic catalytic activity, are emerging promising candidates batteries. Herein, some recent developments atomically summarized, including transition metal non‐transition sites. Moreover, various synthetic strategies, characterization methods, relationship between active site structures RR activity/Zn–CO battery performance introduced. Finally, challenges perspectives also proposed future development ADMCs

Language: Английский

Citations

91
Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO2 Valorization DOI
Liqi Qiu, Hongru Li, Liang‐Nian He

et al.

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(16), P. 2225 - 2240

Published: Aug. 3, 2023

ConspectusCO2 conversion to valuable chemicals is effective at reducing CO2 emissions. We previously proposed valorization strategies and developed efficient catalysts address thermodynamic stability kinetic inertness issues related conversion. Earlier, we molecular capture reagents integrate conversion, i.e., in situ transformation. Based on the mechanistic understanding of capture, activation, transformation a level, set out develop heterogeneous by incorporating catalytic units into nanomaterials via immobilization active onto designing with intrinsic sites.In thermocatalytic carbonaceous metal-organic framework (MOF)-based were for nonreductive reductive Novel Cu- Zn-based MOFs carbon-supported Cu prepared successfully applied cycloaddition, carboxylation, carboxylative cyclization reactions CO2, generating cyclic carbonates, carboxyl acids, oxazolidinones as respective target products. Reductive especially functionalization promising strategy produce chemicals, alleviating chemical production that relies petrochemistry. explored hierarchical using organocatalysts regulate reduction triggering catalyst investigation. Introducing multiple sites opens possibilities novel strategies. realized an N-doped Zn complex MOF materials adsorbents catalysts. These nanomaterial-based feature high excellent efficiency act shape-selective some cases due their unique pore structure.Nanomaterial-based are also appealing candidates photocatalytic (PCO2RR) electrocatalytic (ECO2RR), so series hybrid photo-/electrocatalysts metal complexes different matrixes such porous organic polymers (POPs), layers (MOLs), micelles, conducting polymers. By introducing Re-bipyridine Fe-porphyrin POPs regulating structure polymer chain, increased PCO2RR. PCO2RR aqueous solution was Re-bipyridine-containing amphiphilic form micelles nanoreactors. MOLs two metallic centers, Ni-bipyridine site Ni-O node, improve synergistic effect these centers. Sulfylphenoxy-decorated cobalt phthalocyanine (CoPc) cross-linked polypyrrole used cathode, achieving diluted benefiting from adsorption capability polypyrrole. fabricated immobilized 4-(t-butyl)-phenoxy Bi-MOF cathodes promote paired electrolysis 5-hydroxymethylfurfural (HMF) obtained products 2,5-furandicarboxylic acid (FDCA) efficiently.

Language: Английский

Citations

90
Converting CO2 into Value‐Added Products by Cu2O‐Based Catalysts: From Photocatalysis, Electrocatalysis to Photoelectrocatalysis DOI

Chu‐fan Li,

Rui‐tang Guo,

Zhen‐rui Zhang

et al.

Small, Journal Year: 2023, Volume and Issue: 19(19)

Published: Feb. 11, 2023

Abstract Converting CO 2 into value‐added products by photocatalysis, electrocatalysis, and photoelectrocatalysis is a promising method to alleviate the global environmental problems energy crisis. Among semiconductor materials applied in catalytic reduction, Cu O has advantages of abundant reserves, low price friendliness. Moreover, unique adsorption activation properties for , which conducive generation C 2+ through CC coupling. This review introduces basic principles reduction summarizes pathways 1 products. The factors affecting performance are further discussed from perspective reaction environment, medium, novel reactor design. Then, O‐based catalysts summarized several optimization strategies enhance their stability redox capacity discussed. Subsequently, application photocatalytic, electrocatalytic, photoelectrocatalytic described. Finally, opportunities, challenges research directions field presented, guidance its wide fields provided.

Language: Английский

Citations

83
High-loading of well dispersed single-atom catalysts derived from Fe-rich marine algae for boosting Fenton-like reaction: Role identification of iron center and catalytic mechanisms DOI

Kexin Yin,

Lijing Peng, Dongdong Chen

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 336, P. 122951 - 122951

Published: June 2, 2023

Language: Английский

Citations

80
Facilitating Molecular Activation and Proton Feeding by Dual Active Sites on Polymeric Carbon Nitride for Efficient CO2Photoreduction DOI

Xiaoqiang An,

Qingwen Tang,

Huachun Lan

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(46)

Published: Sept. 23, 2022

Photoreduction of CO2 provides an appealing way to alleviate the energy crisis and manage global carbon balance but is limited by high activation rate-limiting proton transfer. We now develop a dual-site strategy for high-efficiency conversion through polarizing molecules at pyridine N vacancies accelerating intermediate protonation protonated adjacent nitrogen on polymeric nitride. Our photocatalysts with atomic-level engineered active sites manifest CO production rate 1835 μmol g-1 h-1 , 183 times higher than pristine bulk Theoretical prediction experimental studies confirm that such excellent performance attributed synergistic effect between vacant in decreasing formation key *COOH intermediates efficient electron transfer relay facilitated defect-induced shallow trap state homogeneous charge mediators.

Language: Английский

Citations

79