Interstitial boron-triggered electron-deficient Os aerogels for enhanced pH-universal hydrogen evolution

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

---

Constructing a Hetero-interface Composed of Oxygen Vacancy-Enriched Co₃O₄ and Crystalline–Amorphous NiFe-LDH for Oxygen Evolution Reaction

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(23), P. 14338 - 14351

Published: Nov. 12, 2021

The development of high-performance electrocatalysts is a highly efficient strategy to optimize the sluggish kinetic property oxygen evolution reaction (OER). Herein, we synthesize kind nickel foam (NF)-supported electrocatalyst composed one-dimensional Co3O4 nanowire as core and two-dimensional NiFe-LDH nanosheet shell (denoted NiFe-60/Co3O4@NF). Fluorine introduced into precursor Co(OH)F Co3O4, which results in improved thermal stability significantly increased regularly distributed vacancies, while electrochemically deposited nanosheets possess crystalline/amorphous hybrid structure. As result, hetero-interface mainly constituting Ni species from contributes interaction between Co Fe facilitates electron transfer. Simultaneously, vacancies coordinatively unsaturated amorphous area also determined, finally completing backtracking. Benefiting these factors, only low overpotentials 221 257 mV are required deliver current densities 100 500 mA cm–2, respectively, with quite small Tafel slope 34.6 dec–1 during OER for well-designed NiFe-60/Co3O4@NF electrocatalyst.

Language: Английский

---

Interfacial electronic modulation by Fe2O3/NiFe-LDHs heterostructures for efficient oxygen evolution at high current density

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 306, P. 121097 - 121097

Published: Jan. 13, 2022

Language: Английский

---

Site-Specified Two-Dimensional Heterojunction of Pt Nanoparticles/Metal–Organic Frameworks for Enhanced Hydrogen Evolution

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(40), P. 16512 - 16518

Published: Oct. 4, 2021

Heterojunction nanostructures usually exhibit enhanced properties in compariosn with their building blocks and are promising catalyst candidates due to combined surface unique interface. Here, for the first time we realized oriented growth of ultrasmall metal nanoparticles (NPs) on metal–organic framework nanosheets (MOF NSs) by precisely regulating reduction kinetics ions solvents. In particular, a rapid leads random distribution NPs MOF NSs, while slow results edge NSs. Impressively, strong synergy between Pt NSs significantly enhances hydrogen evolution reaction (HER) performance, optimal displays HER activities superior those composite commercial Pt/C under both acidic alkaline conditions. Moreover, versatility such has been extended other NPs, as Pd, Ag, Au. We believe this work will promote research interest material design many potential applications.

Language: Английский

---

Pd–PdO Nanodomains on Amorphous Ru Metallene Oxide for High‐Performance Multifunctional Electrocatalysis

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(12)

Published: Jan. 4, 2023

Developing highly efficient multifunctional electrocatalysts is crucial for future sustainable energy pursuits, but remains a great challenge. Herein, facile synthetic strategy used to confine atomically thin Pd-PdO nanodomains amorphous Ru metallene oxide (RuO2 ). The as-synthesized electrocatalyst (Pd2 RuOx-0.5 h) exhibits excellent catalytic activity toward the pH-universal hydrogen evolution reaction (η10 = 14 mV in 1 m KOH, η10 12 0.5 H2 SO4 , and 22 PBS), alkaline oxygen 225 mV), overall water splitting (E10 1.49 V) with high mass operational stability. Further reduction endows material RuOx-2 promising activity, evidenced by halfway potential, four-electron selectivity, poison tolerance. enhanced attributed rational integration of favorable nanostructures, including 1) nanosheet morphology, 2) coexisting defective crystalline phases, 3) multi-component heterostructural features. These structural factors effectively regulate material's electronic configuration adsorption intermediates at active sites energetics.

Language: Английский

---

Graphene‐Supported Atomically Dispersed Metals as Bifunctional Catalysts for Next‐Generation Batteries Based on Conversion Reactions

Advanced Materials, Journal Year: 2021, Volume and Issue: 34(5)

Published: Oct. 22, 2021

Next-generation batteries based on conversion reactions, including aqueous metal-air batteries, nonaqueous alkali metal-O2 and -CO2 metal-chalcogen metal-ion have attracted great interest. However, their use is restricted by inefficient reversible of active agents. Developing bifunctional catalysts to accelerate the reaction kinetics in both discharge charge processes urgently needed. Graphene-, or graphene-like carbon-supported atomically dispersed metal (G-ADMCs) been demonstrated show excellent activity various electrocatalytic making them promising candidates. Different from G-ADMCs for catalysis, which only require high one direction, rechargeable should provide discharging charging. This review provides guidance design fabrication next-generation reactions. The key challenges that prevent conversion, origin G-ADMCs, current principles highly analyzed highlighted each conversion-type battery. Finally, a summary outlook development G-ADMC materials with energy density efficiency are given.

Language: Английский

---

Non‐Covalent Interaction of Atomically Dispersed Cu and Zn Pair Sites for Efficient Oxygen Reduction Reaction

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 32(32)

Published: May 22, 2022

Abstract Dual–single‐atom catalysts with synergistic effect of adjacent atomic metal sites show a great potential for oxygen reduction reaction (ORR). Herein, dynamical synthetic strategy is demonstrated the rational design dual‐atom catalyst ((Zn, Cu) − NC) non‐covalent Cu and Zn as nitrogen‐doped carbon support. Owing to interaction pair sites, (Zn, NC exhibits significant performances ORR, surpassing individual or site. The theoretical calculations reveal that can highly activate linear O 2 molecule via between pairs, providing more effective overlap 3d orbitals 2p orbital. Therefore, ORR activity optimized improvement adsorption configuration energy . Further, both liquid quasi‐solid zinc air batteries cathodes achieve remarkable density stability. This research proposes facile construct single‐atom presents an insightful understanding interplay heteronuclear atoms in catalysts.

Language: Английский

---

Orbital Occupancy and Spin Polarization: From Mechanistic Study to Rational Design of Transition Metal-Based Electrocatalysts toward Energy Applications

ACS Nano, Journal Year: 2022, Volume and Issue: 16(11), P. 17847 - 17890

Published: Oct. 31, 2022

Over the past few decades, development of electrocatalysts for energy applications has extensively transitioned from trial-and-error methodologies to more rational and directed designs at atomic levels via either nanogeometric optimization or modulating electronic properties active sites. Regarding modulation properties, nonprecious transition metal-based materials have been attracting large interest due capability versatile tuning d-electron configurations expressed through flexible orbital occupancy various possible degrees spin polarization. Herein, recent advances in tailoring transition-metal atoms intrinsically enhanced electrocatalytic performances are reviewed. We start with discussions on how polarization can govern essential level processes, including transport electron charge bulk, reactive species adsorption catalytic surface, transfer between centers adsorbed as well reaction mechanisms. Subsequently, different techniques currently adopted structures discussed particular emphasis theoretical rationale practical achievements. also highlight promises recently established computational design approaches developing applications. Lastly, discussion is concluded perspectives current challenges future opportunities. hope this review will present beauty structure–activity relationships catalysis sciences contribute advance conversion

Language: Английский

---

Recent advances in metal-organic framework-based electrode materials for supercapacitors: A review

Journal of Energy Storage, Journal Year: 2023, Volume and Issue: 62, P. 106934 - 106934

Published: March 18, 2023

Language: Английский

---

CoN nanoparticles anchored on ultra-thin N-doped graphene as the oxygen reduction electrocatalyst for highly stable zinc-air batteries

Carbon, Journal Year: 2022, Volume and Issue: 196, P. 347 - 353

Published: April 27, 2022

Language: Английский

---