Au3+ Species-Induced Interfacial Activation Enhances Metal–Support Interactions for Boosting Electrocatalytic CO2 Reduction to CO DOI

Xiaochen Sun,

Kun Yuan,

Jun‐Hao Zhou

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 12(2), P. 923 - 934

Published: Dec. 30, 2021

The interfacial interactions between the metal and support play a crucial role in electrocatalytic CO2 reduction reaction (CO2RR). In order to promote strong metal–support (SMSIs) of interface, herein, we developed novel synthetic strategy that utilized deposited Au3+ species induce Au–CeO2 interface activation by electrochemical pretreatment. This unique configuration made Au nanoparticles partially be encapsulated CeO2 generate fraction surface with positive charges. obtained catalyst exhibited significantly enhanced selectivity activity CO2RR CO high Faradaic efficiency about 95% under wide potential range from −0.7 −1.0 V. superior performance was attributed activated over which abundant Auδ+ oxygen vacancies generated SMSIs could then accelerate formation *COOH intermediate CO2RR. extended other supports including carbon ZrO2. existence strengthened (MSIs) Faradic obviously higher than catalysts prepared traditional NaBH4 method thus gave new catalytic insights for developing robust supported gold nanocatalysts CO-related important heterogeneous reactions.

Language: Английский

Metal Sites in Zeolites: Synthesis, Characterization, and Catalysis DOI
Qiang Zhang, Shiqin Gao, Jihong Yu

et al.

Chemical Reviews, Journal Year: 2022, Volume and Issue: 123(9), P. 6039 - 6106

Published: Sept. 1, 2022

Zeolites with ordered microporous systems, distinct framework topologies, good spatial nanoconfinement effects, and superior (hydro)thermal stability are an ideal scaffold for planting diverse active metal species, including single sites, clusters, nanoparticles in the framework-associated sites extra-framework positions, thus affording metal-in-zeolite catalysts outstanding activity, unique shape selectivity, enhanced recyclability processes of Brønsted acid-, Lewis metal-catalyzed reactions. Especially, thanks to advances zeolite synthesis characterization techniques recent years, zeolite-confined (denoted as metal@zeolite composites) have experienced rapid development heterogeneous catalysis, owing combination merits both intrinsic properties. In this review, we will present developments strategies incorporating tailoring zeolites advanced identification location, distribution, coordination environment species zeolites. Furthermore, catalytic applications demonstrated, emphasis on composites hydrogenation, dehydrogenation, oxidation Finally, point out current challenges future perspectives precise synthesis, atomic level identification, practical application catalyst system.

Language: Английский

Citations

314

S‐Scheme Co9S8@Cd0.8Zn0.2S‐DETA Hierarchical Nanocages Bearing Organic CO2 Activators for Photocatalytic Syngas Production DOI

Bo Su,

Mei Zheng, Wei Lin

et al.

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(15)

Published: March 1, 2023

Abstract Delicate modulations of CO 2 activation and charge carrier separation/migration are challenging, yet imperative to augment photoreduction efficiency. Herein, by supporting diethylenetriamine (DETA)‐functionalized Cd 0.8 Zn 0.2 S nanowires on the exterior surface hollow Co 9 8 polyhedrons, hierarchical @Cd S‐DETA nanocages fabricated as an S‐scheme photocatalyst for reducing protons produce syngas (CO H ). The amine groups strengthen adsorption , while “nanowire‐on‐nanocage” heterostructure with interface boosts separation transfer photoinduced charges. Employing Co(bpy) 3 2+ a cocatalyst, optimal effectively produces in rates 70.6 18.6 µmol h −1 (i.e., 4673 1240 g ), respectively, affording apparent quantum efficiency 9.45% at 420 nm, which is highest value under comparable conditions. Ultraviolet photoelectron spectroscopy, Kelvin probe, electron spin resonance confirm S‐schematic charge‐transfer process photocatalyst. key COOH * species responsible ‐to‐CO reduction detected in‐situ diffuse reflectance infrared Fourier transform spectroscopy endorsed density functional theory calculations, thus possible mechanism proposed.

Language: Английский

Citations

269

Towards the development of the emerging process of CO2heterogenous hydrogenation into high-value unsaturated heavy hydrocarbons DOI
Jian Wei,

Ruwei Yao,

Yu Han

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(19), P. 10764 - 10805

Published: Jan. 1, 2021

This review covers recent developments in the synthesis of α-olefins and aromatics from CO 2 hydrogenation via direct indirect routes.

Language: Английский

Citations

254

Coverage-driven selectivity switch from ethylene to acetate in high-rate CO2/CO electrolysis DOI
Pengfei Wei, Dunfeng Gao, Tianfu Liu

et al.

Nature Nanotechnology, Journal Year: 2023, Volume and Issue: 18(3), P. 299 - 306

Published: Jan. 12, 2023

Language: Английский

Citations

158

Understanding the Structure–Activity Relationships in Catalytic Conversion of Polyolefin Plastics by Zeolite-Based Catalysts: A Critical Review DOI

Zhongwen Dong,

Wenjun Chen,

Keqing Xu

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(24), P. 14882 - 14901

Published: Nov. 23, 2022

Polyolefins, the largest used commodity plastics in world, find extensive application many fields. However, most end up landfills or incineration, leading to severe ecological crises, environmental pollution, and serious resource waste problems. As representatives on chemical upcycling of polyolefin fuels bulk/fine chemicals, catalytic cracking hydrocracking based zeolite metal/zeolite composite catalysts are considered effective paths due their large capacity strong adaptability existing petrochemical equipment. After an overview reaction mechanisms pyrolysis cracking, this review aims comprehensively discuss influence catalyst structure (acidity, pore structure, morphology) activity, selectivity, stability particularly emphasizing importance for matching acidity target product formation. Subsequently, structure–activity relationship between metal site zeolite's acid is also discussed. In end, emerging opportunities challenges proposed promote a more efficient way upcycling.

Language: Английский

Citations

114

Disentangling the activity-selectivity trade-off in catalytic conversion of syngas to light olefins DOI
Feng Jiao, Bing Bai, Gen Li

et al.

Science, Journal Year: 2023, Volume and Issue: 380(6646), P. 727 - 730

Published: May 18, 2023

Breaking the trade-off between activity and selectivity has been a long-standing challenge in field of catalysis. We demonstrate importance disentangling target reaction from secondary reactions for case direct syngas conversion to light olefins by incorporating germanium-substituted AlPO-18 within framework metal oxide-zeolite (OXZEO) catalyst concept. The attenuated strength catalytically active Brønsted acid sites allows enhancing targeted carbon-carbon coupling ketene intermediates form increasing site density while inhibiting that consume olefins. Thus, light-olefins 83% among hydrocarbons carbon monoxide 85% were obtained simultaneously, leading an unprecedented yield 48% versus current reported yields ≤27%.

Language: Английский

Citations

114

Light olefin synthesis from a diversity of renewable and fossil feedstocks: state-of the-art and outlook DOI Creative Commons
S. A. Chernyak, Massimo Corda,

Jean‐Pierre Dath

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(18), P. 7994 - 8044

Published: Jan. 1, 2022

Light olefins are important feedstocks and platform molecules for the chemical industry. Their synthesis has been a research priority in both academia There many different approaches to of these compounds, which differ by choice raw materials, catalysts reaction conditions. The goals this review highlight most recent trends light olefin perform comparative analysis synthetic routes using several quantitative characteristics: selectivity, productivity, severity operating conditions, stability, technological maturity sustainability. Traditionally, on an industrial scale, cracking oil fractions used produce olefins. Methanol-to-olefins, alkane direct or oxidative dehydrogenation technologies have great potential short term already reached scientific maturities. Major progress should be made field methanol-mediated CO CO2 hydrogenation electrocatalytic reduction is very attractive process long run due low temperature possible use sustainable electricity. application modern concepts such as electricity-driven intensification, looping, management nanoscale catalyst design lead near future more environmentally friendly, energy efficient selective large-scale synthesis.

Language: Английский

Citations

111

Coal measure metallogeny: Metallogenic system and implication for resource and environment DOI
Yong Li, Songqi Pan,

Shuzheng Ning

et al.

Science China Earth Sciences, Journal Year: 2022, Volume and Issue: 65(7), P. 1211 - 1228

Published: May 31, 2022

Language: Английский

Citations

96

Fischer–Tropsch synthesis to olefins boosted by MFI zeolite nanosheets DOI
Chengtao Wang, Fang Wei, Zhiqiang Liu

et al.

Nature Nanotechnology, Journal Year: 2022, Volume and Issue: 17(7), P. 714 - 720

Published: July 1, 2022

Language: Английский

Citations

91

Recent advances on syngas conversion targeting light olefins DOI

Shangqing Zhao,

Haiwei Li, Bo Wang

et al.

Fuel, Journal Year: 2022, Volume and Issue: 321, P. 124124 - 124124

Published: April 8, 2022

Language: Английский

Citations

87