Dual-metal hydroxide with ordering frustrated Lewis pairs for photoactivating CO2 to CO

Wang, Hailian; Zhang, Weining; Lü, Lei; Liu, Depei; Liu, Duanduan; Li, Taozhu; Yan, Shicheng; Zhao, Su; Zou, Zhigang

doi:10.1016/j.apcatb.2020.119639

Cited by 44 publications

(30 citation statements)

References 36 publications

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“…One can surmise that photogenerated electrons and holes would relax to mid‐gap Lewis‐acidic Cu 2+ and Lewis‐basic OH − sites of SFLPs, enhancing its Lewis acidity and Lewis basicity and thereby contribute to significantly increased catalytic rates of 0.5 mol% Cu‐HAP. [ 1 , 2 , 5 , 11 , 12 ]…”

Section: Resultsmentioning

confidence: 99%

“…Gas‐phase photocatalytic CO 2 reduction has attracted global attention; it aims to reduce CO 2 into commodity chemicals and fuels exemplified by CO, CH 4 , HCOOH, CH 3 OH, and C 2+ by using resource‐rich, economical, clean, and renewable solar energy. [ 1 ] Surface frustrated Lewis pairs (SFLPs) can activate H 2 and CO 2 molecules due to their ability to form a highly activated structural space for adsorbed molecules. As a result, SFLPs have been implicated in gas‐phase photocatalytic CO 2 hydrogenation to CO, CH 4 , and CH 3 OH.…”

Section: Introductionmentioning

confidence: 99%

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Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

et al. 2021

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Calcium hydroxyphosphate, Ca 10 (PO 4 ) 6 (OH) 2 , is commonly known as hydroxyapatite (HAP). The acidic calcium and basic phosphate/hydroxide sites in HAP can be modified via isomorphous substitution of calcium and/or hydroxide ions to enable a cornucopia of catalyzed reactions. Herein, isomorphic substitution of Ca 2+ ions by Cu 2+ ions especially at very low levels of exchange created new analogs of molecular surface frustrated Lewis pairs (SFLPs) in Cu x Ca 10−x (PO 4 ) 6 (OH) 2 , thereby boosting its performance metrics in heterogeneous CO 2 photocatalytic hydrogenation. In situ Fourier transform infrared spectroscopy characterization and density functional theory calculations provided fundamental insights into the catalytically active SFLPs defined as proximal Lewis acidic Cu 2+ and Lewis basic OH − . The photocatalytic pathway proceeds through a formate reaction intermediate, which is generated by the reaction of CO 2 with heterolytically dissociated H 2 on the SFLPs. Given the wealth of information thus uncovered, it is highly likely that this work will spur the further development of similar classes of materials, leading to the advancement and, ultimately, large-scale application of photocatalytic CO 2 reduction technologies.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

et al. 2021

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“…Firstly, we synthesize the single-crystal ZnSn(OH) 6 cube with exposed (100) facet by the facile hydrothermal method. [57] According to the photocorrosion treatment under 300 W Xe lamp, the light-unstable surface SnÀ OH would be partially removed to produce the unsaturated metal sites (O Vs ) as Lewis acid, H 2 and O 2 are released at the same time. While the lightstable surface ZnÀ OH could be as the inherent Lewis base.…”

Section: Dual-metal Hydroxides With Ordered Flps For Photoactivation Of Co 2 To Form Comentioning

confidence: 99%

“…Step 2: Heterolytic splitting of CO 2 by FLPs with the help of heterolytically cleaved H 2 . Step 3: Regeneration of FLPs and generation of CO and H 2 O under irradiation [57]. Reproduced with permission from Ref [57],.…”

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Inorganic Frustrated Lewis Pairs in Photocatalytic CO₂ Reduction

Zhang

Qin

et al. 2021

ChemPhotoChem

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Carbon dioxide (CO 2 ) conversion and utilization is a potential means to solve the energy crisis and environmental problems in modern times. However, the energy conversion efficiency is still limited by the high barriers in CO 2 activation and conversion. Due to their ability to capture CO 2 , frustrated Lewis pairs (FLPs) have attracted much attention recently. In this Minireview, we first introduce the basic principles and chal-lenges of photocatalytic CO 2 reduction, including different CO 2 reduction reaction pathways, product selectivity and water oxidation kinetics. Subsequently, research progress of FLPs on the activation of CO 2 /H 2 O molecules, charge separation and transfer and the product selectivity are discussed. Finally, the challenges in photocatalytic CO 2 reduction are presented and future development directions are briefly described.

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Unveiling Spin State‐Dependent Micropollutant Removal using Single‐Atom Covalent Triazine Framework

Zhu

Fang

et al. 2023

Adv Funct Materials

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Single‐atom materials, with unique electronic structure and maximized atom utilization, have shown huge application potential in the remediation of emerging organic pollutants (EOPs), but revealing intrinsic reaction mechanisms at spin state level remains a formidable challenge. Herein, a single‐atom Ti‐loaded covalent organic framework (Ti1/CTF) is constructed for two‐stage process that involved adsorption and photocatalytic synergy, and the essential role of the electronic spin state in regulating the intrinsic activity of the material is evidenced. Spin‐polarized Ti1N3/CTF‐10 considerably enhances the adsorption capacity (453.285 µmol g−1) and degradation kinetics (2.263 h−1, 17.0‐fold faster than CTF‐0) for 2,2,4,4'‐tetrehydroxybenzophenone (BP‐2) and provides long‐term stability (93.3% BP‐2 removal in seven cycles) and favorable cost‐effectiveness (4.45 kWh∙m−3 electrical energy per order) in natural water applications. Theoretical calculations and experimental results suggest that the Ti1N3 moieties of single‐atom Ti bonded to pyridine and triazine N induce electron spin‐down polarization near the Fermi energy level of the active site, providing a strong dipole force and motive power for electron transfer. This study provides new insights into the adsorption, activation, and photodegradation of EOPs at the material interface from the electronic spin level and demonstrates promising solutions for water micropollution control.

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Dual-metal hydroxide with ordering frustrated Lewis pairs for photoactivating CO2 to CO

Cited by 44 publications

References 36 publications

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

Inorganic Frustrated Lewis Pairs in Photocatalytic CO₂ Reduction

Unveiling Spin State‐Dependent Micropollutant Removal using Single‐Atom Covalent Triazine Framework

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Dual-metal hydroxide with ordering frustrated Lewis pairs for photoactivating CO2 to CO

Cited by 44 publications

References 36 publications

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO2 Hydrogenation

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO2 Hydrogenation

Inorganic Frustrated Lewis Pairs in Photocatalytic CO2 Reduction

Unveiling Spin State‐Dependent Micropollutant Removal using Single‐Atom Covalent Triazine Framework

Contact Info

Product

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About

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

Construction of New Active Sites: Cu Substitution Enabled Surface Frustrated Lewis Pairs over Calcium Hydroxyapatite for CO₂ Hydrogenation

Inorganic Frustrated Lewis Pairs in Photocatalytic CO₂ Reduction