Atomically Dispersed Catalytic Platinum Anti-Substitutions in Molybdenum Ditelluride DOI

Jun Zhao,

Xiaocang Han, Junxian Li

et al.

Journal of the American Chemical Society, Journal Year: 2025, Volume and Issue: unknown

Published: March 5, 2025

Atomic defects, e.g., vacancies, substitutions, and dopants, play crucial roles in determining the functionalities of two-dimensional (2D) materials, including spin glass, single-photon emitters, energy storage conversion, due to introduction abnormal charge states noncentrosymmetric distortion. In particular, anti-substitutions are regarded as promising topological defect types, which substitution occurs at opposite sites, fundamentally modifying atomic electronic structures pristine lattices. However, fabrication large-scale remains challenging high formation energies complex reaction paths. Here, we propose an approach for synthesizing atomically dispersed Pt defective 1T'-MoTe2 using electrochemical exfoliation-assisted leaching-redeposition (EELR) method. Atomic-resolution scanning transmission electron microscopy (STEM) imaging reveals that atoms substitute Te forming unconventional Mo-Pt bonds. A rich variety anti-substitution configurations coupling with vacancies have been fabricated by controlled conditions. Density functional theory (DFT) calculations suggest preferentially occupy vacancy sites coupled neighboring stabilizing configurations. The Pt-Te complexes exhibit excellent hydrogen evolution reaction, overpotential only 12.9 mV because paired cause redistribution regulate d-band center active suggested DFT. These findings introduce effective engineering 2D presenting new opportunities precise design features targeted catalytic other advanced applications.

Language: Английский

Heteroatom-doped MXenes as electrocatalysts for hydrogen evolution reaction: A review on the recent advances, mechanisms and prospects DOI
Abdul Hanan, Muhammad Nazim Lakhan, Rashmi Walvekar

et al.

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 483, P. 149107 - 149107

Published: Jan. 28, 2024

Language: Английский

Citations

52
Defect engineering: the role of cationic vacancies in photocatalysis and electrocatalysis DOI

Wenming Ding,

Shengbo Yuan, Yang Yang

et al.

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(44), P. 23653 - 23682

Published: Jan. 1, 2023

Defect engineering is an effective strategy to control the performance of photocatalyst and electrocatalyst. This review highlights key role cationic vacancy from aspects synthesis methods, testing techniques applications.

Language: Английский

Citations

42
Design and regulation of defective electrocatalysts DOI
Yiqiong Zhang, Jingjing Liu, Yangfan Xu

et al.

Chemical Society Reviews, Journal Year: 2024, Volume and Issue: unknown

Published: Jan. 1, 2024

This review focuses on the synthesis and characterization of defective electrocatalysts, internal correlation between defects catalytic activity, development application electrocatalysts in various fields.

Language: Английский

Citations

23
Iron Molybdenum Sulfide‐Supported Ultrafine Ru Nanoclusters for Robust Sulfion Degradation‐Assisted Hydrogen Production DOI
Jiahui Wang, Min Zhou, Rong Fu

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(27)

Published: March 5, 2024

Abstract Electrocatalytic hydrogen evolution and (S 2− ) recycling present promising strategies for cost‐effective production simultaneous removal of environmental pollutants. However, the advancement this technology is hindered by limited availability affordable, efficient, stable catalysts. Herein, study synthesizes ultrafine ruthenium (Ru) nanoclusters on a substrate iron molybdenum sulfide (FeMo‐S) nanosheets, creating new heterointerface catalyst (FeMo‐S/Ru) reaction (HER) sulfion oxidation (SOR). Experimental theoretical calculations suggest that strong electron interactions between Ru FeMo‐S substrate, optimizing *H adsorption promoting HER activity one side while facilitating sulfur intermediates other side, effectively catalyzing SOR. Additionally, assembled electrocatalytic coupling system with FeMo‐S/Ru displays an ultralow cell voltage 0.57 V at 100 mA cm −2 , achieving high Faradaic efficiencies (>96%) H 2 production, also exhibiting remarkable durability over 1 month (838 h). This work paves way development highly efficient durable supported catalysts, enabling energy‐saving environmentally friendly recycling.

Language: Английский

Citations

21
Interfacial Design of Ti3C2Tx MXene/Graphene Heterostructures Boosted Ru Nanoclusters with High Activity Toward Hydrogen Evolution Reaction DOI Creative Commons
Xu Yu, Yong Li, Chengang Pei

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(22)

Published: March 29, 2024

Abstract The development of a cost‐competitive and efficient electrocatalyst is both attractive challenging for hydrogen production by evolution reaction (HER). Herein, facile glycol reduction method to construct Ru nanoclusters coupled with hierarchical exfoliated‐MXene/reduced graphene oxide architectures (Ru‐E‐MXene/rGA) reported. structure, formed the self‐assembly oxides, can effectively prohibit self‐stacking MXene nanosheets. Meanwhile, formation MXene/rGA interface strongly trap 3+ ions, resulting in uniform distribution within Ru‐E‐MXene/rGA. boosted catalytic activity underlying mechanism during HER process are proved density functional theory. Ru‐E‐MXene/rGA exhibits overpotentials 42 62 mV at 10 mA cm −2 alkaline acidic electrolytes, respectively. small Tafel slope charge transfer resistance ( R ct ) values elucidate its fast dynamic behavior. cyclic voltammetry (CV) curves chronoamperometry test confirm high stability These results demonstrate that coupling heterostructure represents an strategy constructing MXene‐based catalysts enhanced activity.

Language: Английский

Citations

17
Enhanced Photocatalytic Efficiency Through Oxygen Vacancy‐Driven Molecular Epitaxial Growth of Metal–Organic Frameworks on BiVO4 DOI Open Access

Yan Xin,

Jian Tian, Xianqiang Xiong

et al.

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

Published: Jan. 19, 2025

Abstract Efficient charge separation at the semiconductor/cocatalyst interface is crucial for high‐performance photoelectrodes, as it directly influences availability of surface charges solar water oxidation. However, establishing strong molecular‐level connections between these interfaces to achieve superior interfacial quality presents significant challenges. This study introduces an innovative electrochemical etching method that generates a high concentration oxygen vacancy sites on BiVO 4 surfaces (Ov‐BiVO ), enabling interactions with oxygen‐rich ligands MIL‐101. reduces formation energy and promotes conformal growth . The Ov‐BiVO /MIL‐101 composite exhibits ideal interface, achieving impressive photocurrent density 5.91 mA cm −2 1.23 V RHE , along excellent stability. high‐performing photoanode enables unbiased tandem device /MIL‐101‐Si cell system, solar‐to‐hydrogen efficiency 4.33%. integration mitigates states enhances internal electric field, facilitating migration photogenerated holes into MIL‐101 overlayer. process activates highly efficient Fe catalytic sites, which effectively adsorb molecules, lowering barrier oxidation improving kinetics. Further studies confirm broad applicability vacancy‐induced molecular epitaxial in various MOFs, offering valuable insights defect engineering optimizing enhancing photocatalytic activity.

Language: Английский

Citations

4
Modulating Carrier Oxygen Vacancies to Enhance Strong Oxide‐Support Interaction in IrO2/Nb2O5‐x Catalysts for Promoting Acidic Oxygen Evolution Reaction DOI

Yun Wu,

Chuanming Guo,

Rui Yao

et al.

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

Published: Sept. 2, 2024

Abstract Given the pronounced dissolution of electrocatalysts in acidic environments, quest for effective oxygen evolution reaction (OER) suitable proton exchange membrane (PEM) water electrolyzers persists as a formidable challenge. In this investigation, catalysts are synthesized by creating vacancies within various metal oxides (Nb 2 O 5‐x , Ta ZrO 2‐x TiO ) through plasma‐assisted method, thereby facilitating immobilization IrO onto these defect‐rich surfaces. The findings unveil that /Nb manifests reduced overpotentials during OER, achieving an overpotential down to 225 mV@10 mA cm −2 coupled with outstanding durability at multicurrent densities exceeding 200 h, attributed strong oxide‐support interaction (SOSI) between catalyst and Nb substrate. Density functional theory (DFT) computations uncover intensified binding affinities thus modulating central energy levels Ir's d orbitals toward favorable OER conditions, consequently bolstering electrocatalytic activity stability composite catalyst. Furthermore, employing PEM electrolyzer anode enables consistent operation 1000 Ir content only 0.2852 mg consumption 4.34 kWh Nm −3 H . This achievement substantially lowers cost hydrogen production US$ 0.96 per kilogram, underscoring its potential practical applications.

Language: Английский

Citations

12
Promoting Polysulfide Redox Reactions through Electronic Spin Manipulation DOI Creative Commons
Jing Yu, Chen Huang, Oleg Usoltsev

et al.

ACS Nano, Journal Year: 2024, Volume and Issue: 18(29), P. 19268 - 19282

Published: July 9, 2024

Catalytic additives able to accelerate the lithium–sulfur redox reaction are a key component of sulfur cathodes in batteries (LSBs). Their design focuses on optimizing charge distribution within energy spectra, which involves refinement and occupancy electronic density states. Herein, beyond distribution, we explore role spin configuration polysulfide adsorption properties catalytic activity additive. We showcase importance this parameter by generating polarization through defect engineering approach based introduction Co vacancies surface CoSe nanosheets. show change electron state increasing number unpaired electrons with aligned spins. This local rearrangement enhances adsorption, reducing activation Li–S reactions. As result, more uniform nucleation growth Li2S an accelerated liquid–solid conversion LSB obtained. These translate into exhibiting capacities up 1089 mA h g–1 at 1 C 0.017% average capacity loss after 1500 cycles, 5.2 cm–2, 0.16% decay per cycle 200 cycles high loading cells.

Language: Английский

Citations

10
Transition Metal Carbonitride MXenes Anchored with Pt Sub-Nanometer Clusters to Achieve High-Performance Hydrogen Evolution Reaction at All pH Range DOI Creative Commons

Zhihao Lei,

Sajjad Ali, CI Sathish

et al.

Nano-Micro Letters, Journal Year: 2025, Volume and Issue: 17(1)

Published: Jan. 31, 2025

Transition metal carbides, known as MXenes, particularly Ti3C2Tx, have been extensively explored promising materials for electrochemical reactions. However, transition carbonitride MXenes with high nitrogen content reactions are rarely reported. In this work, incorporated Pt-based electrocatalysts, ranging from single atoms to sub-nanometer dimensions, hydrogen evolution reaction (HER). The fabricated Pt clusters/MXene catalyst exhibits superior HER performance compared the single-atom-incorporated MXene and commercial Pt/C in both acidic alkaline electrolytes. optimized sample shows low overpotentials of 28, 65, 154 mV at a current densities 10, 100, 500 mA cm-2, small Tafel slope 29 dec-1, mass activity 1203 mgPt-1 an excellent turnover frequency 6.1 s-1 electrolyte. Density functional theory calculations indicate that can be attributed enhanced active sites, increased surface groups, faster charge transfer dynamics, stronger electronic interaction between MXene, resulting absorption/desorption toward better HER. This work demonstrates may candidates various catalytic by incorporating or clusters.

Language: Английский

Citations

1
Rapid Joule-Heating fabrication of oxygen vacancies and anchor of Ru clusters onto BiVO4 for greatly enhanced photocatalytic N2 fixation DOI

Guangmin Ren,

Zehui Zhao,

Zizhen Li

et al.

Journal of Catalysis, Journal Year: 2023, Volume and Issue: 428, P. 115147 - 115147

Published: Sept. 27, 2023

Language: Английский

Citations

20