Heterojunction Engineering of Multinary Metal Sulfide‐Based Photocatalysts for Efficient Photocatalytic Hydrogen Evolution

Advanced Materials, Год журнала: 2023, Номер 36(11)

Опубликована: Дек. 2, 2023

Photocatalytic hydrogen evolution (PHE) via water splitting using semiconductor photocatalysts is an effective path to solve the current energy crisis and environmental pollution. Heterojunction photocatalysts, containing two or more semiconductors, exhibit better PHE rates than those with only one owing altered band alignment at interface stronger driving force for charge separation. Traditional binary metal sulfide (BMS)-based heterojunction such as CdS, MoS

Язык: Английский

---

Interfacial engineering of CoP/CoS2 heterostructure for efficiently electrocatalytic pH-universal hydrogen production

Journal of Colloid and Interface Science, Год журнала: 2023, Номер 652, С. 989 - 996

Опубликована: Авг. 23, 2023

Язык: Английский

---

RuO₂–CeO₂ Lattice Matching Strategy Enables Robust Water Oxidation Electrocatalysis in Acidic Media via Two Distinct Oxygen Evolution Mechanisms

ACS Catalysis, Год журнала: 2024, Номер 14(5), С. 3298 - 3307

Опубликована: Фев. 15, 2024

The discovery of acid-stable and highly active electrocatalysts for the oxygen evolution reaction (OER) is crucial in quest high-performance water-splitting technologies. Herein, a heterostructured RuO2–CeO2 electrocatalyst was constructed by using lattice-matching strategy. interfacial Ru–O–Ce bridge structure provided channel electron transfer between Ru Ce, creating lattice stress that distorts local RuO2. resulting catalyst exhibited attractive stability with negligible decay after 1000 h OER 0.5 M H2SO4, along high activity an overpotential only 180 mV at 10 mA cm–2. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), differential electrochemical mass spectrometry (DEMS), density functional theory (DFT) calculations were used to reveal interface noninterface RuO2 sites enabled oxide path mechanism (OPM) enhanced adsorbate (AEM-plus), respectively, during OER. simultaneous independent pathways accessible matching guides improved design acidic media.

Язык: Английский

---

Local Electronic Structure Modulation of Interfacial Oxygen Vacancies Promotes the Oxygen Activation Capacity of Pt/Ce_1–xM_xO_2−δ

ACS Catalysis, Год журнала: 2024, Номер 14(8), С. 5936 - 5948

Опубликована: Апрель 3, 2024

The asymmetric oxygen vacancies on the surface of doped oxides and at interface between metal oxide are commonly regarded as real active sites for molecular activation reaction, owing to their unique electronic perturbation properties. However, essential rules modulating local structure promote capacity still ambiguous. In this work, a series interfacial vacancy sites, Pt/Ce–Ov–M (Ov, vacancy, M = Y, La, Pr, Nd), with different coordination environments were constructed based Pt/Ce0.95M0.05O2−δ materials. experimental data theoretical calculation results prove that site can capture electrons from Pt d-bands d- f-bands, acting an electron enrichment center. elevated d-band center upward Fermi level significantly boost transfer unoccupied π2p* orbital O2, achieving O2 through π-electron feedback mechanism. Remarkably, Pt/Ce–Ov–Y in Pt/Ce0.95Y0.05O2−δ highest delocalized density exhibited best behaviors catalytic activity aerobic oxidation 5-hydroxymethylfurfural. This work reveals over metal-oxide catalysts is highly dependent d/f-orbital valence-electron modulation, providing more insights into effect vacancy-localized performance.

Язык: Английский

---

Modulation of the electronic structure of CoP by surface and interface codoping boosts electrocatalytic oxygen evolution reaction

International Journal of Hydrogen Energy, Год журнала: 2023, Номер 51, С. 914 - 921

Опубликована: Ноя. 20, 2023

Язык: Английский

---

Enhancement of Nitrate‐to‐Ammonia on Amorphous CeO_x‐Modified Cu via Tuning of Active Hydrogen Supply

Advanced Energy Materials, Год журнала: 2023, Номер 14(7)

Опубликована: Дек. 22, 2023

Abstract The electrochemical nitrate reduction reaction (NO 3 RR) is an environment‐friendly and promising alternative to the conventional Haber–Bosch ammonia synthesis process, which a complex process of proton‐coupled electron transfer. Hereon, amorphous CeO x support introduced construct Cu/a‐CeO heterostructure prepared provide sufficient *H synergistically catalyze NO RR. achieves maximum yield 1.52 mmol h −1 mg cat . In flow cell, NH reaches 17.93 at 1 A cm −2 , exceeds most state‐of‐the‐art catalysts. situ X‐ray diffraction (XRD) in Raman observe that catalyst undergoes structural reconfiguration under operating conditions, thus confirming Cu 2 O not true active center catalytic process. Furthermore, characterizations density functional theory (DFT) calculations demonstrate modulates electronic structure overcomes higher potential barrier required for decomposition water on Cu, greatly facilitates hydrolysis provides H‐coverage rate hydrogenation − realizing dynamic equilibrium between production consumption hydrogen. This component design strategy centered opens up new pathway

Язык: Английский

---

Electron spin-states reconfiguration induced by alternating temperature gradient for boosting photocatalytic hydrogen evolution on hollow core-shell FeS2/CuCo2O4 Z-scheme heterostructure

Nano Energy, Год журнала: 2024, Номер 124, С. 109483 - 109483

Опубликована: Март 11, 2024

Язык: Английский

---

Rational Design of Multiple Heterostructures with Synergistic Effect for Efficient and Stable Hydrogen Evolution Toward Industrial Alkaline Water Splitting

Advanced Functional Materials, Год журнала: 2024, Номер 34(37)

Опубликована: Апрель 21, 2024

Abstract Electrocatalytic hydrogen evolution reaction (HER) via alkaline water splitting holds great promise for industrial clean production but is frustrated by limited catalytic activity and inferior stability under high current density. Elaborate manipulating of heterostructure on robust electrodes essential challenging accelerating HER kinetics with durability. Herein, a nickel mesh electrode, offering mechanical stability, directly engineered layers multiple heterostructures (r‐Mn–Ni/CoP) facile one‐pot electrodeposition followed surface reconstruction strategy. The abundant composed crystalline CoP, NiP, amorphous region, additional Mn doping considerably manipulate the electronic structure optimized charge transfer; while in situ surface‐reconstructed hydrophilic nanoflakes enable rapid wetting active sites to electrolyte. Consequently, r‐Mn–Ni/CoP requires only 134 mV overpotential at density 100 mA cm −2 , superior monophasic undoped samples, majority reported catalysts. Remarkably, an electrolyzer cathode demonstrates extraordinary voltage 1.734 V 300 stable operation 800 h. finding provides feasible strategy fabrication nonprecious‐metal‐based electrocatalysts toward electrolysis.

Язык: Английский

---

In Situ Reconstruction to Surface Sulfide Adsorbed Metal Scaffold for Enhanced Electrocatalytic Hydrogen Evolution Activity

Advanced Energy Materials, Год журнала: 2024, Номер 14(23)

Опубликована: Март 26, 2024

Abstract Transition‐metal‐based compounds have been intensively explored as efficient electrocatalysts for hydrogen evolution reaction (HER). Feasible reconstruction to the real active sites, which is yet be identified, endows promotion of HER activity. Here, it reported that incoming S coordinates and anion vacancies prompt structural S‐doped Co 3 O 4 on carbon cloth (S‐Co /CC) during HER. A list in situ studies reveals sites are “metallic surface‐adparticles” system embracing metallic scaffold dilute coverage coordinated δ+ . Reaction mechanism exploration illustrates interfacial perimeters between moieties considerably facilitate adsorption H*, improve kinetics water dissociation, consequently promote The exemplified sulfide‐mediated topotactic transformation strategy extended preparation S, Fe codoped Ni(OH) 2 (S‐NiFe/CC) a bifunctional electrocatalyst. assembled exchange membrane electrolyzer achieves current density 1.0 cm −2 at 1.72 V, showing excellent capability catalyzing overall splitting ampere level. This study, feasible enables facile identify would inspire development other electrochemical hydrogenation reaction.

Язык: Английский

---

Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications

Advanced Science, Год журнала: 2024, Номер 11(33)

Опубликована: Июль 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

Язык: Английский

---