Broad Light Absorption and Multichannel Charge Transfer Mediated by Topological Surface State in CdS/ZnS/Bi₂Se₃ Nanotubes for Improved Photocatalytic Hydrogen Production

Advanced Functional Materials, Год журнала: 2024, Номер 34(46)

Опубликована: Июль 1, 2024

Abstract Semiconductor heterojunctions have garnered extensive interest in photocatalytic hydrogen generation, yet the limited light absorption and charge transfer efficiencies still restrict performance. The topological insulator has unique surface states high‐mobility electrons, demonstrating significant potential for enhancing photocatalysis. Herein, a ternary photocatalyst based on insulator, which CdS ZnS nanoparticles are grown Bi 2 Se 3 nanotube, is prepared efficient photocatalysis driven by state first time. Under simulated solar irradiation, CdS/ZnS/Bi nanotubes display robust production rate of 7.13 mmol h −1 g , 69.2 times comparable to many CdS‐based photocatalysts. hollow structure, cooperative bandgap excitations three components endow hybrids with wide response harvest energy. Meanwhile, multichannel facilitated internal electric fields within effectively suppresses recombination photogenerated carriers. This mechanism maintains high concentration stable electrons resulting highly production. work provides new inspiration designing heterojunction photocatalysts insulators high‐efficiency solar‐driven energy conversion.

Язык: Английский

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Insights into Operating Conditions on Electrocatalytic CO₂ Reduction

Advanced Energy Materials, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

Abstract Electrocatalytic CO 2 reduction (CO RR) is rapidly emerging as a promising sustainable strategy for transforming into valuable fuels and chemical feedstocks, crucial step toward carbon‐neutral society. The efficiency, selectivity, stability of RR are heavily influenced by the chosen catalyst operating conditions used. Despite substantial advances in development catalysts, there scarcity comprehensive reviews focusing on influence different environments performance. This review offers detailed examination internal external environmental control strategies designed to enhance efficiency. fundamental reaction mechanisms through situ operational techniques, paired with theoretical analyses, discussed while also identifying key challenges future research directions technology. By delivering overview current state field, this highlights critical role control, mechanistic insights, practical considerations needed successful commercialization

Язык: Английский

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Tuning Transition Metal 3d Spin state on Single‐atom Catalysts for Selective Electrochemical CO₂ Reduction

Advanced Materials, Год журнала: 2025, Номер unknown

Опубликована: Март 13, 2025

Abstract Tuning transition metal spin states potentially offers a powerful means to control electrocatalyst activity. However, implementing such strategy in electrochemical CO 2 reduction (CO R) is challenging since rational design rules have yet be elucidated. Here we show how the addition of P dopants ferromagnetic element (Fe, Co, and Ni) single‐atom catalyst (SAC) can shift its state. For instance, with Fe SAC, enable switch from low state ( d x2‐ y2 0 , z2 xz yz 1 xy ) Fe‐N 4 high x2‐y2 3 ‐P. This studied using suite characterization efforts, including X‐ray absorption spectroscopy (XAS), electron resonance (ESR) spectroscopy, superconducting quantum interference device (SQUID) measurements. When used for R, SAC ‐P active sites yields > 90% Faradaic efficiency over wide potential window ≈530 mV maximum partial current density ≈600 mA cm −2 . Density functional theory calculations reveal that 3+ exhibits enhanced back donation via / ‐π* bond, which enhances * COOH adsorption promotes formation. Taken together, results intentionally tuned boost R performance.

Язык: Английский

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Boosting Formate Production in Electrocatalytic CO₂ Reduction on Bimetallic Catalysts Enriched with In–Zn Interfaces

ACS Nano, Год журнала: 2024, Номер 18(52), С. 35749 - 35757

Опубликована: Дек. 18, 2024

We present an effective strategy for developing the dispersing strong-binding metal In on surface of weak-binding Zn, which modulates binding energy reaction intermediates and further facilitates efficient conversion CO2 to formate. The In-Zn interface (In-Zn2) benefits from formation active sites through favorable orbital interactions, leading a Faradaic efficiency 82.7% formate partial current density 12.39 mA cm-2, along with stable performance over 15 h at -1.0 V versus reversible hydrogen electrode. Both in situ Fourier transform infrared spectroscopy functional theory calculations show that bimetallic catalyst can deliver superior *OCHO intermediate, thereby fundamentally accelerating addition, exposed promotes capture activation molecules dynamics within significantly reduce barrier associated generation HCOO-, thus augmenting selectivity catalytic activity generation.

Язык: Английский

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Sequentially Regulating Potential‐Determining Step for Lowering CO₂ Electroreduction Overpotential over Te‐Doped Bi Nanotips

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(36)

Опубликована: Июнь 19, 2024

Electrocatalytic conversion of CO

Язык: Английский

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Modulation of Topological Order in Structural Unit of Nitrides for Enhanced Electrosynthesis of Nitrile

Advanced Functional Materials, Год журнала: 2025, Номер unknown

Опубликована: Янв. 5, 2025

Abstract The electrochemical oxidation of amines has emerged as a promising alternative to traditional energy‐intensive industrial processes for the green synthesis nitriles, and rational design efficient electrocatalysts is crucial due sluggish reaction kinetics. Herein, it reported that modulating topological order within same structural unit can boost catalytic activity electrooxidation benzylamine benzonitrile (BOR). Using nickel nitride model, Cu atoms are introduced into pristine N─Ni framework, inducing change in units resulting formation Ni 3 CuN with an antiperovskite structure. As result, exhibits 2‐fold enhancement BOR compared N, despite fact coordination polyhedra both almost identical. Theoretical calculations demonstrate modulation strategy successfully weakens Ni─N bonding interactions, induces downward shift d‐band centers, optimizes desorption products, which ultimately contributes more superior electrocatalytic CuN. This work provides new perspective on developing advanced through modulation.

Язык: Английский

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Topological quantum materials in catalysis

Journal of Materials Chemistry A, Год журнала: 2025, Номер unknown

Опубликована: Янв. 1, 2025

Let's quantum: topological quantum materials offer high electron mobility, stable surface states, and resistance to contamination, making them ideal candidates for next-generation heterogeneous catalysts.

Язык: Английский

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Efficient Conversion of CO₂ to Ethanol by Utilizing the Topological Surface States of Rare-Earth Cuprates

Nano Letters, Год журнала: 2025, Номер unknown

Опубликована: Фев. 5, 2025

The design of high-performance catalysts for the CO2 reduction reaction (CO2RR) remains a significant challenge in advancing conversion and storage technologies. In this study, we explored novel application topological materials CO2RR, with focus on production high-value C2+ products. Among 14 lanthanum cuprates, Pr2CuO4 was identified as promising candidate due to its robust surface states (TSS) potential selectivity Electrocatalytic experiments demonstrated excellent stable selectivity, achieving over 67% ethanol current density up 220 mA cm–2. Detailed analysis revealed strong interactions between C p orbital key intermediates Cu dx2–y2 dz2 orbitals, which are primary contributors TSS. These significantly enhanced charge transfer along desired pathway, indicating that interplay orbitals TSS-contributing could be pivotal developing new paradigms catalyst by leveraging effects.

Язык: Английский

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Strong interaction between plasmon and topological surface state in Bi ₂ Se ₃ /Cu _{2- x} S nanowires for solar-driven photothermal applications

Science Advances, Год журнала: 2025, Номер 11(11)

Опубликована: Март 12, 2025

Developing high-performance photothermal materials and unraveling the underlying mechanism are essential for applications. Here, performance improved by strong interaction between plasmon topological surface state (TSS) is demonstrated in Bi 2 Se 3 /Cu 2- x S nanowires. This hybrid, which Cu nanosheets were grown on nanowires, leverages resonance TSS-induced optical property, generating wide efficient light absorption. A series of tests reveals coupling, hot electron injection, plasmon-induced hole relaxation within hybrids, endowing with excellent performance. By integrating hybrids into a hydrogel thermoelectric module, evaporator achieves remarkable water evaporation rate 3.67 kilograms per square meter hour solar-to-vapor efficiency 95.2%, maximum output power 1.078 watts under simulated sunlight irradiation. Moreover, conical mirror was introduced to device, greatly enhances without additional energy input.

Язык: Английский

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Synergistic Effect of Topological Semimetal TiSi and Plasmonic Cu for Enhanced Photoelectrocatalytic Water Splitting of TiO₂ Nanorod Array

Inorganic Chemistry, Год журнала: 2025, Номер unknown

Опубликована: Март 29, 2025

Developing high-efficiency and low-cost catalysts for PEC water splitting is vital solving the issues of energy consumption, environmental pollution, global warming. In this study, we designed prepared a composite photoanode TiO2/TiSi/Cu by depositing topological semimetal TiSi film plasmonic Cu nanoparticles onto TiO2 nanorod array. Due to synergistic effect bands SPR Cu, exhibits significantly enhanced optical absorption in visible-light region. Under wavelength (λ) > 420 nm light irradiation, photocurrent density reaches 4.46 mA cm-2 at 1.9 V vs RHE, about 17.84 times that pure TiO2. The carrier lifetime prolonged from 25.04 ns 31.13 TiO2/TiSi/Cu. Furthermore, demonstrates good long-term cyclic stability, with an average hydrogen production rate 8.12 μmol h-1. Our results indicate effective strategy enhance performance This approach could be applied other catalysts, providing new opportunities developing novel efficient catalysts.

Язык: Английский

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