Rh/Cr₂O₃ and CoO_x Cocatalysts for Efficient Photocatalytic Water Splitting by Poly (Triazine Imide) Crystals

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(37)

Опубликована: Май 11, 2023

In situ photo-deposition of both Pt and CoOx cocatalysts on the facets poly (triazine imide) (PTI) crystals has been developed for photocatalytic overall water splitting. However, undesired backward reaction (i.e., formation) noble surface is a spontaneously down-hill process, which restricts their efficiency to run splitting reaction. Herein, we demonstrate that could be largely promoted by decoration Rh/Cr2 O3 as H2 O2 evolution cocatalysts, respectively. Results reveal dual greatly extract charges from bulk surface, while cocatalyst dramatically restrains reaction, achieving an apparent quantum (AQE) 20.2 %

Язык: Английский

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Decade Milestone Advancement of Defect-Engineered g-C3N4 for Solar Catalytic Applications

Nano-Micro Letters, Год журнала: 2024, Номер 16(1)

Опубликована: Янв. 4, 2024

Over the past decade, graphitic carbon nitride (g-C

Язык: Английский

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Defect and nanostructure engineering of polymeric carbon nitride for visible-light-driven CO2 reduction

Chinese Journal of Structural Chemistry, Год журнала: 2024, Номер 43(3), С. 100245 - 100245

Опубликована: Фев. 5, 2024

Язык: Английский

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Interlayer Spacing Regulation by Single‐Atom Indium^δ+–N₄ on Carbon Nitride for Boosting CO₂/CO Photo‐Conversion

Advanced Functional Materials, Год журнала: 2023, Номер 33(35)

Опубликована: Май 17, 2023

Abstract Simultaneous optimization on bulk photogenerated‐carrier separation and surface atomic arrangement of catalyst is crucial for reactivity CO 2 photo‐reduction. Rare studies capture the detail that, better than in‐plane regulation, interlayer‐spacing regulation may significantly influence carrier transport bulk‐catalyst thereby affecting its photo‐reduction in g ‐C 3 N 4 . Herein, through a single atom‐assisted thermal‐polymerization process, single‐atom In‐bonded N‐atom (In δ + –N ) (002) crystal planes originally constructed. This In reduces interplanar spacing by electrostatic adsorption, which enhances carriers greatly promotes photoreduction. The photo‐conversion performance this resulted modified superior to other atom loaded carbon nitride catalysts. Moreover, adsorption , *COOH formation energy, optimizes reaction path. It achieves remarkable 398.87 µmol −1 h yield rate, 0.21% apparent quantum efficiency, nearly 100% selectivity without any cocatalyst or sacrificial agent. Through d modulation atom, study provides ground‐breaking insight enhancement from double‐gain view structural control ‐reduction photocatalysts.

Язык: Английский

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Enhancing polyol/sugar cascade oxidation to formic acid with defect rich MnO2 catalysts

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Июль 26, 2023

Oxidation of renewable polyol/sugar into formic acid using molecular O2 over heterogeneous catalysts is still challenging due to the insufficient activation both and organic substrates on coordination-saturated metal oxides. In this study, we develop a defective MnO2 catalyst through coordination number reduction strategy enhance aerobic oxidation various polyols/sugars acid. Compared common MnO2, tri-coordinated Mn in displays electronic reconstruction surface oxygen charge state rich vacancies. These vacancies create more Mnδ+ Lewis site together with nearby as base sites. This combined structure behaves much like Frustrated pairs, serving facilitate O2, well C-C C-H bonds. As result, shows high catalytic activity (turnover frequency: 113.5 h-1) yield (>80%) comparable noble for glycerol oxidation. The system further extended other excellent performance.

Язык: Английский

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Atomic Cobalt–Silver Dual-Metal Sites Confined on Carbon Nitride with Synergistic Ag Nanoparticles for Enhanced CO₂ Photoreduction

ACS Nano, Год журнала: 2023, Номер 17(12), С. 11869 - 11881

Опубликована: Июнь 8, 2023

Photocatalytic reduction of CO2 to value-added solar fuels is great significance alleviate the severe environmental and energy crisis. Herein, we report construction a synergistic silver nanoparticle catalyst with adjacent atomic cobalt-silver dual-metal sites on P-doped carbon nitride (Co1Ag(1+n)-PCN) for photocatalytic reduction. The optimized photocatalyst achieves high CO formation rate 46.82 μmol gcat-1 70.1% selectivity in solid-liquid mode without sacrificial agents, which 2.68 2.18-fold compared that exclusive single-atom (Ag1-CN) site (Co1Ag1-PCN) photocatalysts, respectively. closely integrated situ experiments density functional theory calculations unravel electronic metal-support interactions (EMSIs) Ag nanoparticles Ag-N2C2 Co-N6-P promote adsorption CO2* COOH* intermediates form CH4, as well boost enrichment transfer photoexcited electrons. Moreover, atomically dispersed Co-Ag SA serve fast-electron-transfer channel while act electron acceptor enrich separate more photogenerated This work provides general platform delicately design high-performance catalysts highly efficient conversion.

Язык: Английский

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Noble‐Metal‐Free Single‐ and Dual‐Atom Catalysts for Artificial Photosynthesis

Advanced Materials, Год журнала: 2023, Номер 36(22)

Опубликована: Май 13, 2023

Abstract Artificial photosynthesis enables direct solar‐to‐chemical energy conversion aimed at mitigating environmental pollution and producing solar fuels chemicals in a green sustainable approach, efficient, robust, low‐cost photocatalysts are the heart of artificial systems. As an emerging new class cocatalytic materials, single‐atom catalysts (SACs) dual‐atom (DACs) have received great deal current attention due to their maximal atom utilization unique photocatalytic properties, whereas noble‐metal‐free ones impart abundance, availability, cost‐effectiveness allowing for scalable implementation. This review outlines fundamental principles synthetic methods SACs DACs summarizes most recent advances (Co, Fe, Cu, Ni, Bi, Al, Sn, Er, La, Ba, etc.) (CuNi, FeCo, InCu, KNa, CoCo, CuCu, based on non‐noble metals, confined arsenal organic or inorganic substrates (polymeric carbon nitride, metal oxides, sulfides, metal–organic frameworks, carbon, acting as versatile scaffolds solar‐light‐driven reactions, including hydrogen evolution, dioxide reduction, methane conversion, synthesis, nitrogen fixation, peroxide production, remediation. The concludes with challenges, opportunities, future prospects photosynthesis.

Язык: Английский

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Enhancing photocatalytic CO2 reduction with TiO2-based materials: Strategies, mechanisms, challenges, and perspectives

Environmental Science and Ecotechnology, Год журнала: 2023, Номер 20, С. 100368 - 100368

Опубликована: Дек. 16, 2023

The concentration of atmospheric CO

Язык: Английский

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Recent Progress of Single‐Atom Photocatalysts Applied in Energy Conversion and Environmental Protection

Small, Год журнала: 2023, Номер 19(22)

Опубликована: Фев. 28, 2023

Abstract Photocatalysis driven by solar energy is a feasible strategy to alleviate crises and environmental problems. In recent years, significant progress has been made in developing advanced photocatalysts for efficient solar‐to‐chemical conversion. Single‐atom catalysts have the advantages of highly dispersed active sites, maximum atomic utilization, unique coordination environment, electronic structure, which become research hotspot heterogeneous photocatalysis. This paper introduces potential supports, preparation, characterization methods single‐atom detail. Subsequently, fascinating effects on three critical steps photocatalysis (the absorption incident light produce electron‐hole pairs, carrier separation migration, interface reactions) are analyzed. At same time, applications conversion protection (CO 2 reduction, water splitting, N fixation, organic macromolecule reforming, air pollutant removal, degradation) systematically summarized. Finally, opportunities challenges discussed. It hoped that this work can provide insights into design, synthesis, application promote development high‐performance photocatalytic systems.

Язык: Английский

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Single-Atom Ni Supported on TiO₂ for Catalyzing Hydrogen Storage in MgH₂

Journal of the American Chemical Society, Год журнала: 2024, Номер 146(15), С. 10432 - 10442

Опубликована: Март 18, 2024

As an efficient and clean energy carrier, hydrogen is expected to play a key role in future systems. However, hydrogen-storage technology must be safe with high density, which difficult achieve. MgH2 promising solid-state material owing its large capacity (7.6 wt %) excellent reversibility, but large-scale utilization restricted by slow hydrogen-desorption kinetics. Although catalysts can improve the kinetics of MgH2, they reduce capacity. Single-atom maximize atom ratio number interfacial sites boost catalytic activity, while easy aggregation at temperatures limits further application. Herein, we designed single-atom Ni-loaded TiO2 catalyst superior thermal stability activity. The optimized 15wt%-Ni0.034@TiO2 reduced onset dehydrogenation temperature 200 °C. At 300 °C, H2 released absorbed 4.6 % within 5 min 6.53 10 s, respectively. apparent activation energies hydrogenation were 64.35 35.17 kJ/mol H2, Even after 100 cycles dehydrogenation, there was still retention rate 97.26%. effect attributed highly synergistic activity Ni, numerous oxygen vacancies, multivalent Tix+ support, Ni plays dominant role, accelerating electron transfer between Mg2+ H– weakening Mg–H bonds. This work paves way for materials practical unitization also extends application catalysis high-temperature reactions.

Язык: Английский

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