Novel Two-Dimensional Metal Organic Frameworks: High-Performance Bifunctional Electrocatalysts for OER/ORR DOI
Xiaofei Wei, Shoufu Cao,

Huakai Xu

et al.

ACS Materials Letters, Journal Year: 2022, Volume and Issue: 4(10), P. 1991 - 1998

Published: Sept. 18, 2022

For the development of energy storage and conversion, it is essential to explore high performance bifunctional catalysts with oxygen reduction evolution reaction (ORR OER). Two-dimensional (2D) metal–organic frameworks (MOFs) abundant exposed active sites have great potential as catalyst materials electrocatalytic activity. Herein, a sequence 2D MOF (TMN2O2, TM = Cr, Mn, Fe, Co, Ni, Cu, Zn) structures 2,3,6,7,10,11-hexahydroxytriphenylene 2,3,6,7,10,11-triphenylenehexamine were designed investigated for their catalytic in ORR OER by using density functional theory. Calculation results reveal that TMN2O2 (TM Ni) superior thermodynamic electrochemical stability during process. Based on water molecule activation free calculations, CoN2O2 structure exhibits low overpotential values 0.33 0.30 V, respectively. The activity OER/ORR can be attributed moderate adsorption interaction key intermediates. valence orbital contribution Co-3dz2 critical adjusting *OOH intermediate, resulting enhancing both OER.

Language: Английский

Regulation methods for the Zn/electrolyte interphase and the effectiveness evaluation in aqueous Zn-ion batteries DOI
Libei Yuan, Junnan Hao, Chun‐Chuan Kao

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(11), P. 5669 - 5689

Published: Jan. 1, 2021

The working principles of interphase strategies to enhance Zn reversibility are discussed. effectiveness evaluation techniques, including electrochemical methods, characterization measurements, and computational simulations, proposed.

Language: Английский

Citations

482
Modulating Built‐In Electric Field via Variable Oxygen Affinity for Robust Hydrogen Evolution Reaction in Neutral Media DOI

Ling-Ling Zhai,

Xiaojie She, Lyuchao Zhuang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(14)

Published: Jan. 24, 2022

Work function strongly impacts the surficial charge distribution, especially for metal-support electrocatalysts when a built-in electric field (BEF) is constructed. Therefore, studying correlation between work and BEF crucial understanding intrinsic reaction mechanism. Herein, we present Pt@CoOx electrocatalyst with large difference (ΔΦ) strong BEF, which shows outstanding hydrogen evolution activity in neutral medium 4.5-fold mass higher than 20 % Pt/C. Both experimental theoretical results confirm interfacial redistribution induced by thus subtly optimizing hydroxide adsorption energy. This not only provides fresh insights into mechanism but also proposes new design principles toward efficient production medium.

Language: Английский

Citations

244
Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution DOI Creative Commons
Yinghao Li, Chun‐Kuo Peng, Huimin Hu

et al.

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: March 3, 2022

Abstract Developing high-performance electrocatalysts for hydrogen evolution reaction (HER) is crucial sustainable production, yet still challenging. Here, we report boron-modulated osmium (B-Os) aerogels with rich defects and ultra-fine diameter as a pH-universal HER electrocatalyst. The catalyst shows the small overpotentials of 12, 19, 33 mV at current density 10 mA cm −2 in acidic, alkaline, neutral electrolytes, respectively, well excellent stability, surpassing commercial Pt/C. Operando X-ray absorption spectroscopy that interventional interstitial B atoms can optimize electron structure B-Os stabilize Os active sites an electron-deficient state under realistic working conditions, simultaneously reveals catalytic mechanisms electrolytes. functional theory calculations also indicate introducing tailor electronic Os, resulting reduced water dissociation energy improved adsorption/desorption behavior hydrogen, which synergistically accelerate HER.

Language: Английский

Citations

232
Understanding H2 Evolution Electrochemistry to Minimize Solvated Water Impact on Zinc‐Anode Performance DOI Creative Commons
Fuhua Yang, Jodie A. Yuwono, Junnan Hao

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(45)

Published: Sept. 20, 2022

H2 evolution is the reason for poor reversibility and limited cycle stability with Zn-metal anodes, impedes practical application in aqueous zinc-ion batteries (AZIBs). Here, using a combined gas chromatography experiment computation, it demonstrated that primarily originates from solvated water, rather than free water without interaction Zn2+ . Using linear sweep voltammetry (LSV) salt electrolytes, evidenced to occur at more negative potential zinc reduction because of high overpotential against on Zn metal. The hypothesis tested and, glycine additive reduce confirmed "parasitic" side reactions are suppressed anode. This electrolyte suppress evolution, corrosion, give uniform deposition Zn|Zn Zn|Cu cells. It Zn|PANI (highly conductive polyaniline) full cells exhibit boosted electrochemical performance 1 M ZnSO4 -3 electrolyte. concluded this new understanding electrochemistry can be used design relatively low-cost safe AZIBs large-scale energy storage.

Language: Английский

Citations

221
Engineering Platinum–Cobalt Nano‐alloys in Porous Nitrogen‐Doped Carbon Nanotubes for Highly Efficient Electrocatalytic Hydrogen Evolution DOI
Song Lin Zhang, Xue Feng Lu, Zhi‐Peng Wu

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(35), P. 19068 - 19073

Published: June 17, 2021

Abstract Highly efficient electrocatalysts are essential for the production of green hydrogen from water electrolysis. Herein, a metal‐organic framework‐assisted pyrolysis‐replacement‐reorganization approach is developed to obtain ultrafine Pt‐Co alloy nanoparticles (sub‐10 nm) attached on inner and outer shells porous nitrogen‐doped carbon nanotubes (NCNT) with closed ends. During thermal reorganization, migration nano‐alloys both surfaces ensures maximized exposure active sites while maintaining robust attachment matrix. Density functional theory calculations suggest nearly thermodynamically‐neutral free energy adsorption intermediates diversified induced by alloying, thus resulting in great promotion intrinsic activity towards evolution reaction (HER). Benefiting delicate structural design compositional modulation, optimized Pt 3 Co@NCNT electrocatalyst manifests outstanding HER superior stability acidic alkaline media.

Language: Английский

Citations

208
Design and Synthesis of Hollow Nanostructures for Electrochemical Water Splitting DOI Creative Commons
Min Yang,

Cai Hong Zhang,

Nianwu Li

et al.

Advanced Science, Journal Year: 2022, Volume and Issue: 9(9)

Published: Jan. 18, 2022

Abstract Electrocatalytic water splitting using renewable energy is widely considered as a clean and sustainable way to produce hydrogen an ideal fuel for the future. Electrocatalysts are indispensable elements large‐scale electrolysis, which can efficiently accelerate electrochemical reactions occurring at both ends. Benefitting from high specific surface area, well‐defined void space, tunable chemical compositions, hollow nanostructures be applied promising candidates of direct electrocatalysts or supports loading internal external electrocatalysts. Herein, some recent progress in structural design micro‐/nanostructured materials advanced summarized. First, principles corresponding strategies toward highly effective oxygen/hydrogen evolution highlighted. Afterward, overview current reports about with diverse architectural designs functionalities given, including single‐shelled, multi‐shelled, open features heterostructured based on hosts. Finally, future research directions discussed personal perspectives.

Language: Английский

Citations

207
Progress and perspective for conversion of plastic wastes into valuable chemicals DOI
Kai Zheng, Yang Wu,

Zexun Hu

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 52(1), P. 8 - 29

Published: Dec. 5, 2022

We divide the up-to-date techniques into two categories: technologies executed under violent conditions and mild conditions, we present a timely summary of mechanism bond cleavage in plastic waste to produce valuable chemicals.

Language: Английский

Citations

198
A clicking confinement strategy to fabricate transition metal single-atom sites for bifunctional oxygen electrocatalysis DOI Creative Commons
Zhao Chang-xin, Jia‐Ning Liu, Juan Wang

et al.

Science Advances, Journal Year: 2022, Volume and Issue: 8(11)

Published: March 16, 2022

Rechargeable zinc-air batteries call for high-performance bifunctional oxygen electrocatalysts. Transition metal single-atom catalysts constitute a promising candidate considering their maximum atom efficiency and high intrinsic activity. However, the fabrication of atomically dispersed transition sites is highly challenging, creating need new design strategies synthesis methods. Here, clicking confinement strategy proposed to efficiently predisperse transitional atoms in precursor directed by click chemistry ensure successful construction abundant sites. Concretely, cobalt-coordinated porphyrin units are covalently clicked on substrate cobalt affording Co-N-C electrocatalyst. The electrocatalyst exhibits impressive electrocatalytic performances with an activity indicator Δ E 0.79 V. This work extends approach prepare efficient electrocatalysis inspires methodology precise catalytic materials.

Language: Английский

Citations

195
Amorphous/Crystalline Heterostructure Transition-Metal-based Catalysts for High-Performance Water Splitting DOI
Yangping Zhang, Fei Gao,

Dongqiong Wang

et al.

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 475, P. 214916 - 214916

Published: Oct. 31, 2022

Language: Английский

Citations

194
Recent Advances on Transition Metal Dichalcogenides for Electrochemical Energy Conversion DOI
Xin Wu, Huabin Zhang, Jian Zhang

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(38)

Published: Aug. 18, 2021

Abstract Transition metal dichalcogenides (TMDCs) hold great promise for electrochemical energy conversion technologies in view of their unique structural features associated with the layered structure and ultrathin thickness. Because inert basal plane accounts majority a TMDC's bulk, activation sites is necessary to fully exploit intrinsic potential TMDCs. Here, recent advances on TMDCs‐based hybrids/composites greatly enhanced activity are reviewed. After summary synthesis TMDCs different sizes morphologies, comprehensive in‐plane strategies described detail, mainly including in‐plane‐modification‐induced phase transformation, surface‐layer modulation, interlayer modification/coupling. Simultaneously, underlying mechanisms improved activities highlighted. Finally, strategic evaluation further research directions featured. This work would shed some light future design trends functional materials energy‐related applications.

Language: Английский

Citations

169