Amide Covalent Bonding Engineering in Heterojunction for Efficient Solar-Driven CO₂ Reduction

ACS Nano, Год журнала: 2023, Номер 17(20), С. 20560 - 20569

Опубликована: Окт. 4, 2023

Inefficient charge separation and slow interfacial reaction dynamics significantly hamper the efficiency of photocatalytic CO2 reduction. Herein, a facile EDC/NHS-assisted linking strategy was developed to enhance in heterojunction photocatalysts. Using this approach, we successfully synthesized amide-bonded carbon quantum dot-g-C3N4 (CQD-CN) The formation amide covalent bonds between CN CQDs CN-CQD facilitates efficient carrier migration, adsorption, activation. Exploiting these advantages, photocatalysts exhibit high selectivity with CO CH4 evolution rates 79.2 2.7 μmol g-1 h-1, respectively. These are about 1.7 3.6 times higher than those CN@CQD bulk CN, Importantly, demonstrate exceptional stability, even after 12 h continuous testing. presence COOH* signal is identified as crucial intermediate species conversion CO. This study presents bonding engineering for developing high-performance solar-driven reduction CO2.

Язык: Английский

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Photoelectron “Bridge” in Van Der Waals Heterojunction for Enhanced Photocatalytic CO₂ Conversion Under Visible Light

Advanced Materials, Год журнала: 2023, Номер 35(38)

Опубликована: Июнь 26, 2023

Constructing Van der Waals heterojunction is a crucial strategy to achieve excellent photocatalytic activity. However, in most heterojunctions synthesized by ex situ assembly, electron transfer encounters huge hindrances at the interface between two components due large spacing and potential barrier. Herein, phosphate-bridged of cobalt phthalocyanine (CoPc)/tungsten disulfide (WS2 ) bridged phosphate (xCoPc-nPO4- -WS2 designed prepared traditional wet chemistry method. By introducing small molecule into CoPc WS2 , creates an "bridge", resulting compact combination eliminating space Therefore, (PO4- bridge can serve as efficient channel efficiently transmit photoelectrons from under excited states. These are captured catalytic central Co2+ subsequently convert CO2 molecules CO CH4 products, achieving 17-fold enhancement on 3CoPc-0.6PO4- sample compared that pure . Introducing "bridge" create provides new perspective designing photocatalysts for reduction valuable products.

Язык: Английский

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Synergistic Interplay of Dual‐Active‐Sites on Metallic Ni‐MOFs Loaded with Pt for Thermal‐Photocatalytic Conversion of Atmospheric CO₂ under Infrared Light Irradiation

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(48)

Опубликована: Окт. 11, 2023

Abstract Infrared light driven photocatalytic reduction of atmospheric CO 2 is challenging due to the ultralow concentration (0.04 %) and low energy infrared light. Herein, we develop a metallic nickel‐based metal–organic framework loaded with Pt (Pt/Ni‐MOF), which shows excellent activity for thermal‐photocatalytic conversion H even under irradiation. The open Ni sites are beneficial capture activate , while photogenerated electrons dominate dissociation on sites. Simultaneously, thermal results in spilling dissociated sites, where adsorbed thermally reduced CH 4 . synergistic interplay dual‐active‐sites renders Pt/Ni‐MOF record efficiency 9.57 % at 940 nm converting enables procurement be independent emission sources, improves trace by eliminating media regeneration molecular release.

Язык: Английский

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A nonmetallic plasmonic catalyst for photothermal CO2 flow conversion with high activity, selectivity and durability

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Фев. 10, 2024

Abstract The meticulous design of active sites and light absorbers holds the key to development high-performance photothermal catalysts for CO 2 hydrogenation. Here, we report a nonmetallic plasmonic catalyst Mo N/MoO - x nanosheets by integrating localized surface plasmon resonance effect with two distinct types Leveraging synergism dual sites, H molecules can be simultaneously adsorbed activated on N atom O vacancy, respectively. Meanwhile, this noble-metal-free signifies its promising ability convert photon energy into heat. Consequently, exhibit remarkable catalytic performance in reverse water-gas shift reaction. Under continuous full-spectrum irradiation (3 W·cm −2 ) duration 168 h, achieve yield rate 355 mmol·gcat −1 ·h flow reactor selectivity exceeding 99%. This work offers valuable insights precise reducing carbon footprints.

Язык: Английский

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Engineering Built‐In Electric Field Microenvironment of CQDs/g‐C₃N₄ Heterojunction for Efficient Photocatalytic CO₂ Reduction

Advanced Science, Год журнала: 2024, Номер 11(28)

Опубликована: Май 10, 2024

Abstract Graphitic carbon nitride (CN), as a nonmetallic photocatalyst, has gained considerable attention for its cost‐effectiveness and environmentally friendly nature in catalyzing solar‐driven CO 2 conversion into valuable products. However, the photocatalytic efficiency of reduction with CN remains low, accompanied by challenges achieving desirable product selectivity. To address these limitations, two‐step hydrothermal‐calcination tandem synthesis strategy is presented, introducing quantum dots (CQDs) forming ultra‐thin CQD/CN nanosheets. The integration CQDs induces distinct work function CN, creating robust interface electric field after combination. This facilitates accumulation photoelectrons region, providing an abundant source reduced electrons process. Remarkably, nanosheets exhibit average yield 120 µmol g −1 , showcasing outstanding selectivity 92.8%. discovery not only presents innovative pathway development high‐performance photocatalysts grounded non‐metallic materials employing but also opens new avenues versatile application prospects environmental protection sustainable cleaning energy.

Язык: Английский

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Crystal Engineering of MOF‐Derived Bimetallic Oxide Solid Solution Anchored with Au Nanoparticles for Photocatalytic CO₂ Reduction to Syngas and C₂ Hydrocarbons

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(21)

Опубликована: Март 20, 2024

Abstract Considering that CO 2 reduction is mostly a multielectron reaction, it necessary for the photocatalysts to integrate multiple catalytic sites and cooperate synergistically achieve efficient photocatalytic various products, such as C hydrocarbons. Herein, through crystal engineering, we designed constructed metal–organic framework‐derived Zr/Ti bimetallic oxide solid solution support, which was confirmed by X‐ray diffraction, electron microscopy absorption spectroscopy. After anchoring Au nanoparticles, composite photocatalyst exhibited excellent performances toward syngas (H production rates of 271.6 260.6 μmol g −1 h ) even hydrocarbons (C H 4 6 6.80 4.05 ). According control experiments theoretical calculations, strong interaction between support nanoparticles found be beneficial binding intermediates reducing reduction, highlighting synergy effect system with active sites.

Язык: Английский

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Optimization of Schottky barrier height and LSPR effect by dual defect induced work function changes for efficient solar-driven hydrogen production

Chemical Engineering Journal, Год журнала: 2024, Номер 490, С. 151822 - 151822

Опубликована: Май 1, 2024

Язык: Английский

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Concentrated solar CO2 reduction in H2O vapour with >1% energy conversion efficiency

Nature Communications, Год журнала: 2024, Номер 15(1)

Опубликована: Июнь 1, 2024

Abstract H 2 O dissociation plays a crucial role in solar-driven catalytic CO methanation, demanding high temperature even for solar-to-chemical conversion efficiencies <1% with modest product selectivity. Herein, we report an oxygen-vacancy (V o ) rich CeO catalyst single-atom Ni anchored around its surface V sites by replacing Ce atoms to promote and achieve effective photothermal reduction under concentrated light irradiation. The photon flux reduces the apparent activation energy CH 4 production prevents from depletion. defects coordinated Ni, significantly capture of charges local phonons at d -impurity orbitals, thereby inducing more activation. presents yield 192.75 µmol/cm /h, efficiency 1.14% selectivity ~100%. mechanistic insights uncovered this study should help further development O-activating catalysts expedite practical utilization technologies.

Язык: Английский

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Photocontrolled heterojunctions constructed from holmium single atom modified Mg_1.2Ti_1.8O₅/g-C₃N₄ with enhanced photocatalytic CO₂ conversion

Energy & Environmental Science, Год журнала: 2024, Номер 17(14), С. 5039 - 5047

Опубликована: Янв. 1, 2024

This work is the first to introduce photocontrolled catalysts into CO 2 RR, and further RE single atom catalysts, aiming optimize photocatalytic performance by utilizing synergistic effect of composites.

Язык: Английский

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Progress in design and preparation of multi-atom catalysts for photocatalytic CO2 reduction

Science China Materials, Год журнала: 2024, Номер 67(2), С. 397 - 423

Опубликована: Янв. 5, 2024

Язык: Английский

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