Coordination Tunes Selectivity: Two‐Electron Oxygen Reduction on High‐Loading Molybdenum Single‐Atom Catalysts

Angewandte Chemie International Edition, Год журнала: 2020, Номер 59(23), С. 9171 - 9176

Опубликована: Март 20, 2020

Single-atom catalysts (SACs) have great potential in electrocatalysis. Their performance can be rationally optimized by tailoring the metal atoms, adjacent coordinative dopants, and loading. However, doing so is still a challenge because of limited synthesis approach insufficient understanding structure-property relationships. Herein, we report new kind Mo SAC with unique O,S coordination high loading over 10 wt %. The isolation local environment was identified high-angle annular dark-field scanning transmission electron microscopy extended X-ray absorption fine structure. SACs catalyze oxygen reduction reaction (ORR) via 2 e- pathway H2 O2 selectivity 95 % 0.10 m KOH. critical role single atoms structure revealed both electrochemical tests theoretical calculations.

Язык: Английский

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Design concept for electrocatalysts

Nano Research, Год журнала: 2021, Номер 15(3), С. 1730 - 1752

Опубликована: Сен. 4, 2021

Язык: Английский

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Understanding the structure-performance relationship of active sites at atomic scale

Nano Research, Год журнала: 2022, Номер 15(8), С. 6888 - 6923

Опубликована: Июнь 14, 2022

Язык: Английский

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Scalable two-step annealing method for preparing ultra-high-density single-atom catalyst libraries

Nature Nanotechnology, Год журнала: 2021, Номер 17(2), С. 174 - 181

Опубликована: Ноя. 25, 2021

Язык: Английский

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Enhanced Photocatalytic H₂O₂ Production over Carbon Nitride by Doping and Defect Engineering

ACS Catalysis, Год журнала: 2020, Номер 10(24), С. 14380 - 14389

Опубликована: Ноя. 24, 2020

Photocatalytic production of H2O2 from the reduction O2 by semiconductor photocatalysts (e.g., graphitic carbon nitride, C3N4) has been regarded as an alternative for small-scale decentralized production. However, efficiency pristine C3N4 is still limited narrow light absorption range and rapid charge recombination. Here, we presented a facile approach to simultaneously enhance promote separation introducing alkali metal dopants N vacancies on C3N4. The introduction successfully broadened range, reduced band gap 2.85 2.63 eV, greatly inhibited synergistic effect doping defect resulted in improvement photocatalytic performance with rate 10.2 mmol/h/g, which 89.5 times that Thus, this work not only gives insights into manipulating processes but also inspires further develop more efficient

Язык: Английский

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Activity Trends and Mechanisms in Peroxymonosulfate‐Assisted Catalytic Production of Singlet Oxygen over Atomic Metal‐N‐C Catalysts

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(41), С. 22513 - 22521

Опубликована: Авг. 13, 2021

Abstract We synthesized a series of carbon‐supported atomic metal‐N‐C catalysts (M‐SACs: M=Mn, Fe, Co, Ni, Cu) with similar structural and physicochemical properties to uncover their catalytic activity trends mechanisms. The peroxymonosulfate (PMS) are Fe‐SAC>Co‐SAC>Mn‐SAC>Ni‐SAC>Cu‐SAC, Fe‐SAC displays the best single‐site kinetic value (1.65×10 5 min −1 mol ) compared other species. First‐principles calculations indicate that most reasonable reaction pathway for 1 O 2 production is PMS→OH*→O*→ ; M‐SACs exhibit moderate near‐average Gibbs free energies in each step have better activity, which key outstanding performance Fe‐SACs. This study gives atomic‐scale understanding fundamental mechanisms PMS‐assisted reactive oxygen species via M‐SACs, thus providing guidance developing organic pollutant degradation.

Язык: Английский

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A Review on Challenges and Successes in Atomic-Scale Design of Catalysts for Electrochemical Synthesis of Hydrogen Peroxide

ACS Catalysis, Год журнала: 2020, Номер 10(14), С. 7495 - 7511

Опубликована: Июнь 10, 2020

Hydrogen peroxide is a valuable chemical oxidant with wide range of applications in variety industrial processes, especially water sanitization. Electrochemical synthesis hydrogen (H2O2) through two-electron oxygen reduction reaction (2e-ORR) or oxidation (2e-WOR) has emerged as an appealing process for onsite production this chemically oxidant. On-site produced H2O2 can be applied wastewater treatment remote locations any where needed oxidizing agent. This Review studies the theoretical efforts understanding challenges catalysis electrochemical well providing design principles more efficient catalyst materials.

Язык: Английский

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Coordination Engineering of Single‐Atom Catalysts for the Oxygen Reduction Reaction: A Review

Advanced Energy Materials, Год журнала: 2020, Номер 11(3)

Опубликована: Ноя. 30, 2020

Abstract Future renewable energy supplies and a sustainable environment rely on many important catalytic processes. Single‐atom catalysts (SACs) are attractive because of their maximum atom utilization efficiency, tunable electronic structures, outstanding performance. Of particular note, transition‐metal SACs exhibit excellent activity selectivity for the oxygen reduction reaction (ORR)—an half in fuel cells metal–air batteries as well portable hydrogen peroxide (H 2 O ) production. Although considerable efforts have been made synthesis ORR, regulation coordination environments thus structures still pose big challenge. In this review, strategies manipulating classified into three categories, including center metal atoms, manipulation surrounding connecting to atom, modification geometric configuration support. Finally, some issues regarding future development ORR raised possible solutions proposed.

Язык: Английский

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An Adjacent Atomic Platinum Site Enables Single‐Atom Iron with High Oxygen Reduction Reaction Performance

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(35), С. 19262 - 19271

Опубликована: Июнь 22, 2021

Abstract The modulation effect has been widely investigated to tune the electronic state of single‐atomic M‐N‐C catalysts enhance activity oxygen reduction reaction (ORR). However, in‐depth study is rarely reported for isolated dual‐atomic metal sites. Now, catalytic activities Fe‐N 4 moiety can be enhanced by adjacent Pt‐N through effect, in which acts as modulator 3d orbitals active site and optimize ORR activity. Inspired this principle, we design synthesize electrocatalyst that comprises /Pt‐N moieties dispersed nitrogen‐doped carbon matrix (Fe‐N @NC) exhibits a half‐wave potential 0.93 V vs. RHE negligible degradation (ΔE 1/2 =8 mV) after 10000 cycles 0.1 M KOH. We also demonstrate not effective optimizing performances Co‐N Mn‐N systems.

Язык: Английский

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Electrocatalysis of Single-Atom Sites: Impacts of Atomic Coordination

ACS Catalysis, Год журнала: 2020, Номер 10(14), С. 7584 - 7618

Опубликована: Июнь 11, 2020

Single metal atoms embedded within select supporting matrices have shown great potential in the development of high-efficiency, low-cost electrocatalysts because maximal atom utilization and mass activity. As single are stabilized by coordination bonds with substrate, strong metal–support interactions can be exploited for ready manipulation electrocatalytic activity selectivity toward target reactions. However, most single-atom catalysts (SACs) prepared pyrolysis contain a wide range structures. Resolving atomic configurations moieties represents critical first step establishment an unambiguous correlation between SAC structure In this Review, we summarize recent progress studies electrocatalysts, focus on impacts sites activities series reactions that important various electrochemical energy technologies, such as hydrogen evolution reaction, oxygen reduction nitrogen CO2 so on. The survey entails SACs, from noble metals (e.g., Pt, Pd, Ru, Ir, Au, etc.) to non-noble Fe, Co, Ni, Cu, etc.), supported variety substrate materials pristine doped carbon, metal, oxide, sulfide, etc.). Finally, Review concludes perspective highlighting promises challenges further SACs context chemistry.

Язык: Английский

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