Atomic-level polarization in electric fields of defects for electrocatalysis DOI Creative Commons
Jie Xu, Xiong‐Xiong Xue, Gonglei Shao

и другие.

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 29, 2023

The thriving field of atomic defect engineering towards advanced electrocatalysis relies on the critical role electric polarization at scale. While this is proposed theoretically, spatial configuration, orientation, and correlation with specific catalytic properties materials are yet to be understood. Here, by targeting monolayer MoS2 rich in defects, we pioneer direct visualization such defects combining electron microscopy differential phase contrast technology. It revealed that asymmetric charge distribution caused facilitates adsorption H*, which originally activates sites for hydrogen evolution reaction (HER). Then, it has been experimentally proven atomic-level fields can enhance HER activity. This work bridges long-existing gap between directly revealing angstrom-scale correlating as-tuned materials; methodology here could also inspire future studies focusing mechanism understanding structure-property-performance relationship.

Язык: Английский

Enlarging the Ni–O Bond Polarizability in a Phosphorene-Hosted Metal–Organic Framework for Boosted Water Oxidation Electrocatalysis DOI
Wenfang Zhai, Ya Chen, Yaoda Liu

и другие.

ACS Nano, Год журнала: 2023, Номер 17(17), С. 17254 - 17264

Опубликована: Авг. 31, 2023

The emerging lattice-oxygen oxidation mechanism (LOM) presents attractive opportunities for breaking the scaling relationship to boost oxygen evolution reaction (OER) with direct OLattice-*O interaction. However, currently LOM-triggering rationales are still debated, and a streamlined physicochemical paradigm is extremely desirable design of LOM-defined OER catalysts. Herein, Ni metal-organic framework/black phosphorene (NiMOF/BP) heterostructure theoretically profiled constructed as catalytic platform LOM-derived studies. It found that p-type BP host can enlarge Ni-O bond polarizability NiMOF through stretching valence declining synergically. Such an enlarged will in principle alleviate lattice confinement benefit LOM pathway performance. As result, optimized NiMOF/BP catalyst exhibits promising performance low overpotential 260 mV at 10 mA cm-2 long-term stability 1 M KOH electrolyte. Both experiment calculation results suggest activated more balanced step barrier catalyst. This research puts forward criterion LOM-scaled electrocatalysts water oxidation.

Язык: Английский

Процитировано

57
Directional Reconstruction of Iron Oxides to Active Sites for Superior Water Oxidation DOI
Haijun Liu, Shuo Zhang, Wenyu Yang

и другие.

Advanced Functional Materials, Год журнала: 2023, Номер 33(43)

Опубликована: Июнь 27, 2023

Abstract Rationally constructing and manipulating the in situ formed catalytically active surface of catalysts remains a tremendous challenge for highly efficient water electrolysis. Herein, an anion cation co‐induced strategy is presented to modulate catalyst dissolution‐redeposition achieve directional reconstruction Zn S co‐doped Fe 2 O 3 4 on iron foams (Zn,S‐Fe ‐Fe /IF), oxygen evolution reaction (OER). Benefiting from Zn, co‐doping presence , directionally reconstructed obtained. The Zn,S‐Fe /IF into FeOOH ‐FeOOH/IF), which leaching promotes dissolution co‐deposition regulates activity obtained FeOOH. Moreover, provides stable site deposition, thus causes more components be formed. Directionally ‐FeOOH/IF outperformes many state‐of‐the‐art OER demonstrates remarkable stability. experimental density functional theory (DFT) calculation results show that introduction Zn‐doped with abundant vacancies through has activated lattice atoms, facilitating process heterojunction following mechanism (LOM) pathway. This work makes stride modulating reconstruction.

Язык: Английский

Процитировано

51
Unlocking power of neighboring vacancies in boosting hydrogen evolution reactions on two-dimensional NiPS3 monolayer DOI Creative Commons

Hyun Gu Han,

Jae Won Choi,

Minsu Son

и другие.

eScience, Год журнала: 2023, Номер 4(3), С. 100204 - 100204

Опубликована: Окт. 16, 2023

This study investigates the effect of defect engineering on catalytic activity a NiPS3 monolayer catalyst for hydrogen evolution reaction (HER). Three different types vacancies basal plane are explored through multi-step mechanism involving dissociative adsorption water molecule and subsequent electrochemical dissociated proton. Co-formation in both Ni S sites is found to be most effective enhancing performance monolayer. A key resource thermodynamics S-substitution-like physisorption vacant site, followed by occupation OH H into elements, boosted NiS di-vacancy configuration with low activation energy barriers. Investigation reveals highest contribution bonding orbitals monolayer-H bond makes it desirable approach transition metal phosphorus chalcogenides high HER activities. Overall, this highlights significance controlled augmenting catalysts HER.

Язык: Английский

Процитировано

50
Unraveling and leveraging in situ surface amorphization for enhanced hydrogen evolution reaction in alkaline media DOI Creative Commons
Qiang Fu, Lok Wing Wong, Fangyuan Zheng

и другие.

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Окт. 13, 2023

Surface amorphization provides electrocatalysts with more active sites and flexibility. However, there is still a lack of experimental observations mechanistic explanations for the in situ process its crucial role. Herein, we propose concept that by reconstructed amorphous surface, metal phosphorus trichalcogenides could intrinsically offer better catalytic performance alkaline hydrogen production. Trace Ru (0.81 wt.%) doped into NiPS3 nanosheets Using electrochemical transmission electron microscopy technique, confirmed occurred on edges critical achieving superior activity. Comprehensive characterizations theoretical calculations reveal primarily stabilized at through formed layer containing bridging S22- species, which can effectively reduce reaction energy barrier. This work emphasizes role suggests potential optimizing activities electrocatalysts.

Язык: Английский

Процитировано

49
Atomic-level polarization in electric fields of defects for electrocatalysis DOI Creative Commons
Jie Xu, Xiong‐Xiong Xue, Gonglei Shao

и другие.

Nature Communications, Год журнала: 2023, Номер 14(1)

Опубликована: Ноя. 29, 2023

The thriving field of atomic defect engineering towards advanced electrocatalysis relies on the critical role electric polarization at scale. While this is proposed theoretically, spatial configuration, orientation, and correlation with specific catalytic properties materials are yet to be understood. Here, by targeting monolayer MoS2 rich in defects, we pioneer direct visualization such defects combining electron microscopy differential phase contrast technology. It revealed that asymmetric charge distribution caused facilitates adsorption H*, which originally activates sites for hydrogen evolution reaction (HER). Then, it has been experimentally proven atomic-level fields can enhance HER activity. This work bridges long-existing gap between directly revealing angstrom-scale correlating as-tuned materials; methodology here could also inspire future studies focusing mechanism understanding structure-property-performance relationship.

Язык: Английский

Процитировано

49