Engineering interfacial sulfur migration in transition-metal sulfide enables low overpotential for durable hydrogen evolution in seawater

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: July 22, 2024

Abstract Hydrogen production from seawater remains challenging due to the deactivation of hydrogen evolution reaction (HER) electrode under high current density. To overcome activity-stability trade-offs in transition-metal sulfides, we propose a strategy engineer sulfur migration by constructing nickel-cobalt sulfides heterostructure with nitrogen-doped carbon shell encapsulation (CN@NiCoS) electrocatalyst. State-of-the-art ex situ / characterizations and density functional theory calculations reveal restructuring CN@NiCoS interface, clearly identifying dynamic migration. The NiCoS stimulates creating vacancies at Ni 3 S 2 -Co 9 8 heterointerface, while migrated atoms are subsequently captured CN via strong C-S bond, preventing sulfide dissolution into alkaline electrolyte. Remarkably, dynamically formed sulfur-doped pairing sites significantly enhances HER activity altering d -band center near Fermi level, resulting low overpotential 4.6 mV 10 mA cm −2 freshwater media, long-term stability up 1000 h. This work thus provides guidance for design high-performance electrocatalyst engineering interfacial atomic

Language: Английский

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Recent Advances and Perspectives on Coupled Water Electrolysis for Energy‐Saving Hydrogen Production

Advanced Science, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 7, 2025

Abstract Overall water splitting (OWS) to produce hydrogen has attracted large attention in recent years due its ecological‐friendliness and sustainability. However, the efficiency of OWS been forced by sluggish kinetics four‐electron oxygen evolution reaction (OER). The replacement OER alternative electrooxidation small molecules with more thermodynamically favorable potentials may fundamentally break limitation achieve production low energy consumption, which also be accompanied value‐added chemicals than or electrochemical degradation pollutants. This review critically assesses latest discoveries coupled various OWS, including alcohols, aldehydes, amides, urea, hydrazine, etc. Emphasis is placed on corresponding electrocatalyst design related mechanisms (e.g., dual hydrogenation N–N bond breaking hydrazine C═N regulation urea inhibit hazardous NCO − NO productions, etc.), along emerging reactions (electrooxidation tetrazoles, furazans, iodide, quinolines, ascorbic acid, sterol, trimethylamine, etc.). Some new decoupled electrolysis self‐powered systems are discussed detail. Finally, potential challenges prospects highlighted aid future research directions.

Language: Английский

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Multi-channel charge transfer in self-supporting B-g-C3Nx/Bi2S3/CdS dual S-scheme heterojunction toward enhanced photothermal-photocatalytic performance

Nano Energy, Journal Year: 2023, Volume and Issue: 120, P. 109164 - 109164

Published: Dec. 5, 2023

Language: Английский

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All-in-one self-floating porous foams as robust heat-blocking layers for efficient photothermal conversion and solar desalination

Science Bulletin, Journal Year: 2023, Volume and Issue: 68(22), P. 2760 - 2768

Published: Sept. 19, 2023

Language: Английский

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Kinetically and Thermodynamically Favorable Ni–Al Layered Double Hydroxide/Ni-Doped Zn_0.5Cd_0.5S S-Scheme Heterojunction Triggering Photocatalytic H₂ Evolution

Inorganic Chemistry, Journal Year: 2023, Volume and Issue: 62(17), P. 6843 - 6850

Published: April 20, 2023

Layered double hydroxide (LDH)-based photocatalysts have attracted more attention in photocatalysis due to their low cost, wide band gaps, and adjustable photocatalytic active sites; however, photogenerated carrier separation efficiency limits efficiency. Herein, a NiAl-LDH/Ni-doped Zn0.5Cd0.5S (LDH/Ni-ZCS) S-scheme heterojunction is rationally designed constructed from kinetically thermodynamically favorable angles. The 15% LDH/1% Ni-ZCS displays comparable hydrogen evolution (PHE) activity with rate of 6584.0 μmol g-1 h-1, which exceeds by ∼6.14- ∼1.73-fold those ZCS 1% Ni-ZCS, respectively, outperforms most the previously reported LDH-based metal sulfide-based photocatalysts. In addition, apparent quantum yield reaches 12.1% at 420 nm. situ X-ray photoelectron spectroscopy, photodeposition, theoretical calculation reveal specific transfer path carriers. On this basis, we propose possible mechanism. fabrication not only accelerates carriers but also decreases activation energy H2 improves redox capacity. Moreover, there are huge amounts hydroxyl groups distributed on surface photocatalysts, highly polar easy combine H2O large dielectric constant form bond, can further accelerate PHE.

Language: Английский

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Activating Fe activity and improving Ni activity via C3N4 substrate in alkaline oxygen evolution catalyzed by Ni-Fe phosphide

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 342, P. 123391 - 123391

Published: Oct. 11, 2023

Language: Английский

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Pauling‐Type Adsorption of O₂ Induced by Heteroatom Doped ZnIn₂S₄ for Boosted Solar‐Driven H₂O₂ Production

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 63(5)

Published: Dec. 12, 2023

Abstract Breaking the trade‐off between activity and selectivity has perennially been a formidable endeavor in field of hydrogen peroxide (H 2 O ) photosynthesis, especially side‐on configuration oxygen (O on catalyst surface will cause cleavage O−O bonds, which drastically hinders H production performance. Herein, we present an atomically heteroatom P doped ZnIn S 4 with tunable adsorption to accelerate ORR kinetics essential for solar‐driven production. Indeed, spectroscopy characterizations (such as EXAFS situ FTIR) DFT calculations reveal that at substitutional interstitial sites, not only optimizes coordination environment Zn active but also facilitates electron transfer sites improves charge density, avoiding breakage bonds reducing energy barriers As result, is regulated from (Yeager‐type) end‐on (Pauling‐type), resulting accelerated 874.94 2107.66 μmol g −1 h . This finding offers new avenue toward strategic tailoring by rational design photocatalyst.

Language: Английский

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Photocatalytic upgrading of 5-hydroxymethylfurfural – aerobic or anaerobic?

Green Chemistry, Journal Year: 2024, Volume and Issue: 26(6), P. 2949 - 2966

Published: Jan. 1, 2024

Aerobic photocatalysis generates ROS to oxidise HMF into DFF and FDCA with co-production of H 2 O that potentially induce over-oxidation. Anaerobic enables ambient oxidation simultaneous HER, or hydrogenation BHMF.

Language: Английский

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Cyanuric Acid-Assisted Synthesis of Hierarchical Amorphous Carbon Nitride Assembled by Ultrathin Oxygen-Doped Nanosheets for Excellent Photocatalytic Hydrogen Generation

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(12), P. 14809 - 14821

Published: March 18, 2024

Amorphous carbon nitride with typical short-range order arrangement as an effective photocatalyst is worth exploring but remains a great challenge because its disordered structure induces severe recombination of photogenerated charge carriers. Herein, for the first time, we demonstrate that hierarchical amorphous (HACN) structural oxygen incorporation can be synthesized via cyanuric acid-assisted melem hydrothermal process, accompanied by freeze-drying and pyrolysis. The complex composed acid exhibiting unique 3D self-supporting skeleton significant phase transformation responsible formation interconnected framework HACN. These features are beneficial to enhance visible light harvesting multiple-reflection effect within architecture consisting more exposed porous nanosheets introducing long band tail absorption. well-designed morphology, state, doping effectively inhibit rapid band-to-band electrons holes facilitate subsequent separation. Accordingly, HACN catalyst exhibits exceptional (λ > 420 nm)-driven photoreduction hydrogen production rate 82.4 μmol h–1, which 21.7 9.5 times higher than those melem-derived crystalline nanotube counterparts, respectively, significantly surpasses most reported nitrides. Our controlling rearrangement in situ supramolecular self-assembly oligomer using directly instructs development highly efficient photocatalysts converting solar energy into fuel.

Language: Английский

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Efficient Charge Separation in Ag/PCN/UPDI Ternary Heterojunction for Optimized Photothermal‐Photocatalytic Performance via Tandem Electric Fields

Small, Journal Year: 2024, Volume and Issue: 20(28)

Published: May 21, 2024

Charge separation driven by the internal electric field is a research hotspot in photocatalysis. However, it remains challenging to accurately control continuously accelerate charge transfer. Herein, strategy of constructing tandem transfer photocatalysts proposed. The plasma field, interface and intramolecular are integrated into Ag/g-C

Language: Английский

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