Concurrent Photocatalytic CO2 Reduction and 1‐Phenylethanol Oxidation Regulated by Chloride Ion‐Capped CdS@ZnxCd1‐xS@ZnS QDs DOI Open Access

Huakang Yang,

Zining Zhang, Yudong Guo

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Abstract Solar‐driven photocatalytic CO 2 reduction coupled with the oxidation of organic compounds to value‐added chemicals is a promising strategy, which can utilize both photogenerated electrons and holes. Here, gradient alloyed CdS@Zn x Cd 1‐x S@ZnS quantum dots (quasi‐Type II band structure) capped Cl − ligands demonstrate great potential in simultaneous conversion 1‐phenylethanol into syngas pinacol. The passivation maximizes exposure surface‐active sites improves their electronic structure, providing prerequisite for efficient execution redox reactions. More importantly, p–π conjugation between chloride‐ion benzene ring provides bridge ultrafast transfer holes, greatly promotes activation Cα─H bond release mass reactive free hydrogen. This process effectively lowers thermodynamic energy barrier reduction, even as excessively high kinetic barriers arising from accumulation excess protons also enable them self‐couple, leading generation (CO ≈ 75 mmol g −1 h ; selectivity 69.86%). work insights future artificial photosynthesis achieve activity cost‐effective storable renewable resources co‐production substances through synergistic oxidation.

Language: Английский

Sustainable photocatalytic hydrogen peroxide production over octonary high-entropy oxide DOI Creative Commons

Hao Ling,

Huacong Sun,

Lisha Lu

et al.

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

Published: Nov. 3, 2024

The direct utilization of solar energy for the artificial photosynthesis hydrogen peroxide (H2O2) provides a reliable approach producing this high-value green oxidant. Here we report on utility high-entropy oxide (HEO) semiconductor as an all-in-one photocatalyst visible light-driven H2O2 production directly from H2O and atmospheric O2 without need any additional cocatalysts or sacrificial agents. This contains eight earth-abundant metal elements (Ti/V/Cr/Nb/Mo/W/Al/Cu) homogeneously arranged within single rutile phase, intrinsic chemical complexity along with presence high density oxygen vacancies endow distinct broadband light harvesting capability. An efficient rate apparent quantum yield 38.8% at 550 nm can be achieved. readily assembled into floating leaves sustained on-site open water resources under natural sunlight irradiation. "all-in-one" enables photocatalytic external agents

Language: Английский

Citations

12
Hollow Stair-Stepping Spherical High-Entropy Prussian Blue Analogue for High-Rate Sodium Ion Batteries DOI
Yifan Zhang, Jiajia Huang,

Linyang Qiu

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(21), P. 27684 - 27693

Published: May 16, 2024

Prussian blue analogues (PBAs) are considered to be one of the most suitable sodium storage materials, especially with introduction high-entropy (HE) concept into their structure further improve various abilities. However, severe agglomeration HEPBA particles still limits fast charging capabilities. Here, an (Nax(FeMnCoNiCu)[Fe(CN)6]y□1–y·nH2O) a hollow stair-stepping spherical has been prepared through chemical etching process traditional cubic HEPBA. Electrochemical characterization (sodium ion battery), kinetic analysis, and COMSOL Multiphysics simulations reveal that nature can greatly diffusion behavior Na+ ions. Moreover, effectively mitigates volume change during SIBs operation, ultimately extending lifespan. Consequently, as-prepared cathode exhibits excellent rate performance (126.5 76.4 mAh g–1 at 0.1 4.0 A g–1, respectively) stable long-term capability (maintaining its 75.6% capacity after 1000 cycles) due unique structure. Furthermore, waste easily recycled prepare more product. This processing method holds great promise for designing nanostructures advanced batteries.

Language: Английский

Citations

10
Tailoring bismuth defects in Bi2WO6 nanosheets for photocatalytic C–H activation DOI Creative Commons
Xinye Li, Luteng Luo, Hele Guo

et al.

Journal of Materials Chemistry A, Journal Year: 2024, Volume and Issue: 12(20), P. 11841 - 11847

Published: Jan. 1, 2024

Tailoring the bismuth defects in ultrathin Bi 2 WO 6 nanosheets can efficiently activate C–H bond toluene to produce benzaldehyde under light irradiation.

Language: Английский

Citations

9
Synthesis Strategies for High Entropy Nanoparticles DOI
Linlin Yang, Ren He,

Jiali Chai

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 30, 2024

Abstract Nanoparticles (NPs) of high entropy materials (HEMs) have attracted significant attention due to their versatility and wide range applications. HEM NPs can be synthesized by fragmenting bulk HEMs or disintegrating recrystallizing them. Alternatively, directly producing in NP form from atomic/ionic/molecular precursors presents a challenge. A widely adopted strategy involves thermodynamically driving formation leveraging the entropic contribution but incorporating strategies limit growth at elevated temperatures used for maximizing entropy. second approach is kinetically drive promoting rapid reactions homogeneous reactant mixtures using highly diluted precursor dissolutions. Additionally, experimental evidence suggests that enthalpy plays role processes moderate temperatures, with energy cost generating additional surfaces interfaces nanoscale stabilizing phase. This review critically assesses various synthesis developed preparation, highlighting key illustrative examples offering insights into underlying mechanisms. Such are critical fine‐tuning conditions achieve specific outcomes, ultimately enabling effective optimized generations these advanced both current emerging applications across scientific technological fields.

Language: Английский

Citations

8
High-Entropy Rock-Salt Surface Layer Stabilizes the Ultrahigh-Ni Single-Crystal Cathode DOI
Zhongxing Xu, Xinghan Chen, Wenguang Fan

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 28, 2024

Single-crystalline Ni-rich layered oxides are one of the most promising cathode materials for lithium-ion batteries due to their superior structural stability. However, sluggish diffusion kinetics and interfacial issues hinder practical applications. These intensify with increasing Ni content in ultrahigh-Ni regime (≥90%), significantly threatening viability single-crystalline strategy oxide cathodes. Herein, by developing a high-entropy coating strategy, we successfully constructed an epitaxial lattice-coherent rock-salt layer (∼3 nm) via Zr Al doping on surface LiNi

Language: Английский

Citations

8
Enigma of Sustainable CO2 Conversion to Renewable Fuels and Chemicals Through Photocatalysis, Electrocatalysis, and Photoelectrocatalysis: Design Strategies and Atomic Level Insights DOI Open Access

Diksha Suri,

Srimanta Das,

Shivani Choudhary

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 2, 2025

Growing global population, escalating energy consumption, and climate change threaten future security. Fossil fuel combustion, primarily coal, oil, natural gas, exacerbates the greenhouse effect driving warming through CO

Language: Английский

Citations

1
Accompanying Bi Clusters as Charge Mediators Effectively Enhance Synergetic Redox of Bi2Sn2O7/ZnIn2S4 S‐Scheme Heterostructure Composites DOI Open Access
Xing Liu, Yu-Chen Su, Yudong Li

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 5, 2025

Abstract Achieving synergistic oxidation and reduction represents a significant challenge in the field of photocatalysis. In this study, hydrothermal/in situ construction Bi atom clusters within 2 Sn O 7 /ZnIn S 4 (BSO/ZIS) heterostructures is reported. These exhibit self‐accelerating charge‐transfer mechanisms facilitated by internal electric fields bonding bridges, resulting highly efficient light absorption capabilities. X‐ray photoelectron spectroscopy (XPS) Kelvin probe force microscopy (KPFM), as well theoretical calculations, indicate that canonical induction promotion electrons holes lowers activation energy CHO* generation, allowing simultaneous CO toluene over catalyst, enhances proton‐coupling electron‐transfer processes, unique reaction mechanism. The reactant, Bi‐Bi (B‐BSO/ZIS) heterostructure achieves rate to 726.3 µmol g −1 h (99.9% selectivity) benzaldehyde 2362.0 (98.0% selectivity), which increases activity 14.6 5.7 times compared pristine ZnIn . This study underscores significance modulating photocatalytic pathway through strategic selection metal reactants, contributing rational design photocatalysts for enhanced adsorption stabilization *H.

Language: Английский

Citations

1
High‐Entropy Layered Double Hydroxides for Efficient Methanol Electrooxidation DOI Open Access
Yuying Wang,

Yihang Hu,

Zhaohui Wu

et al.

Small, Journal Year: 2025, Volume and Issue: 21(11)

Published: Feb. 16, 2025

Abstract The electrocatalytic methanol oxidation reaction (MOR) is considered as an effective method to replace oxygen evolution (OER) for efficient hydrogen production. However, the sluggish kinetics and difficulty of breaking C─H bond Ni‐based catalysts limit further application. Herein, three high‐entropy layered double hydroxides (HELHs), namely ZnNiFeCoV‐HELH, ZnNiFeCoCr‐HELH, ZnNiFeCoAl‐HELH (denoted V‐HELH, Cr‐HELH, Al‐HELH, respectively), are successfully synthesized. Among them, V‐HELH displays lowest potential 1.39 V at 100 mA cm −2 compared Cr‐HELH (1.41 V) Al‐HELH (1.44 V). After five cycles, formate yield maintains over 95% first cycle with excellent stability. Such outstanding performance surpasses that most state‐of‐the‐art MOR reported so far. A series experiments reveal exhibits fastest largest number active Ni 3+ species. Further investigations theoretical calculations prove shows strongest adsorption energy −3.31 eV. introduction vanadium (V) relatively larger tensile strain optimizes d─band center (−0.54 eV) lowers barrier (−1.62 from * CH 3 O 2 O. This work provides new insights rational design electrocatalysts.

Language: Английский

Citations

1
Enthralling Anodic Protection by Molybdate on High‐Entropy Alloy‐Based Electrocatalyst for Sustainable Seawater Oxidation DOI
Sakila Khatun, Kōji Shimizu, Santanu Kumar Pal

et al.

Small, Journal Year: 2024, Volume and Issue: 20(43)

Published: June 25, 2024

Efficient and sustainable seawater electrolysis is still limited due to the interference of chloride corrosion at anode. The designing suitable electrocatalysts one crucial ways boost electrocatalytic activity. However, approach may fall short as achieving high current density often occurs in chlorine evolution reaction (CER)-dominating potential regions. Thereby, apart from developing an OER-active high-entropy alloy-based electrocatalyst, present study also offers a unique way protect anode surface under or by using MoO

Language: Английский

Citations

6
Role of polarized and interfacial built-in electric fields in photocatalysts for enhanced photocatalytic performance DOI

Caiyu Luo,

Chunping Yang,

Jun Xie

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 497, P. 155514 - 155514

Published: Sept. 12, 2024

Language: Английский

Citations

6