Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction DOI
Yizhe Li, Hao Sun,

Longtao Ren

и другие.

Angewandte Chemie International Edition, Год журнала: 2024, Номер 63(28)

Опубликована: Май 9, 2024

The single-atom Fe-N-C catalyst has shown great promise for the oxygen reduction reaction (ORR), yet intrinsic activity is not satisfactory. There a pressing need to gain deeper understanding of charge configuration and develop rational modulation strategies. Herein, we have prepared Fe with co-coordination N O (denoted as Fe-N/O-C) adjacent defect, proposing strategy optimize d-orbital spin-electron filling sites by fine-tuning first coordination shell. Fe-N/O-C exhibits significantly better ORR compared its counterpart commercial Pt/C, much more positive half-wave potential (0.927 V) higher kinetic current density. Moreover, using catalyst, Zn-air battery proton exchange membrane fuel cell achieve peak power densities up 490 1179 mW cm

Язык: Английский

Single‐atom catalysis for carbon neutrality DOI Creative Commons
Ligang Wang, Dingsheng Wang, Yadong Li

и другие.

Carbon Energy, Год журнала: 2022, Номер 4(6), С. 1021 - 1079

Опубликована: Июль 14, 2022

Abstract Currently, more than 86% of global energy consumption is still mainly dependent on traditional fossil fuels, which causes resource scarcity and even emission high amounts carbon dioxide (CO 2 ), resulting in a severe “Greenhouse effect.” Considering this situation, the concept “carbon neutrality” has been put forward by 125 countries one after another. To achieve goals neutrality,” two main strategies to reduce CO emissions develop sustainable clean can be adopted. Notably, these are crucial for synthesis advanced single‐atom catalysts (SACs) energy‐related applications. In review, we highlight unique SACs conversion into high‐efficiency energy, example, through photocatalytic, electrocatalytic, thermal catalytic hydrogenation technologies, convert hydrocarbon fuels (CO, CH 4 , HCOOH, 3 OH, multicarbon [C 2+ ] products). addition, introduce technologies devices replace polluting such as photocatalytic electrocatalytic water splitting produce hydrogen oxygen reduction reaction (ORR) fuel cells. Impressively, several representative examples (including d ‐, ds p f ‐blocks) conversion, H ORR discussed describe methods, characterization, corresponding activity. Finally, review concludes with description challenges outlooks future applications contributing toward neutrality.

Язык: Английский

Процитировано

206

ZnIn2S4-based photocatalysts for photocatalytic hydrogen evolution via water splitting DOI

Xinlong Zheng,

Yiming Song, Yuhao Liu

и другие.

Coordination Chemistry Reviews, Год журнала: 2022, Номер 475, С. 214898 - 214898

Опубликована: Окт. 22, 2022

Язык: Английский

Процитировано

200

What is the Real Origin of the Activity of Fe–N–C Electrocatalysts in the O2 Reduction Reaction? Critical Roles of Coordinating Pyrrolic N and Axially Adsorbing Species DOI
Xu Hu, Suya Chen, Letian Chen

и другие.

Journal of the American Chemical Society, Год журнала: 2022, Номер 144(39), С. 18144 - 18152

Опубликована: Сен. 22, 2022

Fe–N–C electrocatalysts have emerged as promising substitutes for Pt-based catalysts the oxygen reduction reaction (ORR). However, their real catalytic active site is still under debate. The underlying roles of different types coordinating N including pyridinic and pyrrolic in performance require thorough clarification. In addition, how to understand pH-dependent activity another urgent issue. Herein, we comprehensively studied 13 N-coordinated FeNxC configurations corresponding ORR through simulations which mimic realistic electrocatalytic environment on basis constant-potential implicit solvent models. We demonstrate that contributes a higher than N, FeN4C exhibits highest acidic media. Meanwhile, situ transformation *O-FeN4C *OH-FeN4C clarifies origin alkaline These findings can provide indispensable guidelines rational design better durable catalysts.

Язык: Английский

Процитировано

195

Single atomic cobalt electrocatalyst for efficient oxygen reduction reaction DOI Creative Commons
Peng Rao, Daoxiong Wu, Tianjiao Wang

и другие.

eScience, Год журнала: 2022, Номер 2(4), С. 399 - 404

Опубликована: Май 18, 2022

Robust oxygen reduction reaction (ORR) catalysts are essential for energy storage and conversion devices, but their development remains challenging. Herein, we design a single-atom catalyst featuring isolated Co anchored on nitrogen-doped carbon (Co-SAC/NC) via highly efficient “plasma-bombing” strategy. With high loading (up to 2.5 ​wt%), the well-dispersed single atoms in Co-SAC/NC give it robust ORR performance an alkaline medium. It also demonstrates excellent battery when implemented as air-cathode zinc-air (ZAB). Theoretical calculations reveal that Co–N4 moiety experiences “extraction/recovery” structural evolution during process, reaction's rate-determining step is formation of OOH∗ (reaction intermediate). This work provides new strategy designing high-performance ZABs other energy-conversion devices.

Язык: Английский

Процитировано

189

The reformation of catalyst: From a trial-and-error synthesis to rational design DOI
Ligang Wang, Jiabin Wu,

Shunwu Wang

и другие.

Nano Research, Год журнала: 2023, Номер 17(4), С. 3261 - 3301

Опубликована: Сен. 27, 2023

Язык: Английский

Процитировано

183

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

Daijie Deng,

Junchao Qian, Xiaozhi Liu

и другие.

Advanced Functional Materials, Год журнала: 2022, Номер 32(32)

Опубликована: Май 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.

Язык: Английский

Процитировано

152

Carbon‐Based Electrocatalysts for Acidic Oxygen Reduction Reaction DOI Creative Commons

Pengbo Cui,

Linjie Zhao, Yongde Long

и другие.

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(14)

Опубликована: Янв. 16, 2023

Abstract Oxygen reduction reaction (ORR) is vital for clean and renewable energy technologies, which require no fossil fuel but catalysts. Platinum (Pt) the best‐known catalyst ORR. However, its high cost scarcity have severely hindered devices (e.g., cells) large‐scale applications. Recent breakthroughs in carbon‐based metal‐free electrochemical catalysts (C‐MFECs) show great potential earth‐abundant carbon materials as low‐cost electrocatalysts towards ORR acidic media. This article provides a focused, critical review on C‐MFECs media with an emphasis advances structure design synthesis, fundamental understanding of structure‐property relationship electrocatalytic mechanisms, their applications proton exchange membrane cells. Current challenges future perspectives this emerging field are also discussed.

Язык: Английский

Процитировано

148

Movable type printing method to synthesize high-entropy single-atom catalysts DOI Creative Commons
Peng Rao, Yijie Deng, Wenjun Fan

и другие.

Nature Communications, Год журнала: 2022, Номер 13(1)

Опубликована: Авг. 29, 2022

The controllable anchoring of multiple isolated metal atoms into a single support exhibits scientific and technological opportunities, while the synthesis catalysts with remains challenge has been rarely reported. Herein, we present general route for up to eleven metals as highly dispersed single-atom centers on porous nitride-doped carbon supports developed movable type printing method, label them high-entropy catalysts. Various tunable multicomponent are successfully synthesized same method by adjusting only templates carbonization parameters. To prove utility, quinary (FeCoNiCuMn) is investigated oxygen reduction reaction catalyst much more positive activity durability than commercial Pt/C catalyst. This work broadens family opens way investigate efficient compositions.

Язык: Английский

Процитировано

142

Progress in the development of heteroatom-doped nickel phosphates for electrocatalytic water splitting DOI

Yanhui Yu,

Qingrong Chen, Jing Li

и другие.

Journal of Colloid and Interface Science, Год журнала: 2021, Номер 607, С. 1091 - 1102

Опубликована: Сен. 16, 2021

Язык: Английский

Процитировано

115

Hierarchically Ordered Macro–Mesoporous Electrocatalyst with Hydrophilic Surface for Efficient Oxygen Reduction Reaction DOI Open Access
Wen Yao,

Anqian Hu,

Jieting Ding

и другие.

Advanced Materials, Год журнала: 2023, Номер 35(30)

Опубликована: Апрель 18, 2023

Metal-organic frameworks (MOFs) offer versatile templates/precursors to prepare supported metal catalysts. However, the afforded catalysts usually exhibit microporous structures and unsuitable wettability, which will restrict accessibility of active sites in liquid-phase reactions. Herein, an etching-functionalization strategy is developed for construction a tannic-acid-functionalized MOF with unique hollow-wall 3D-ordered macroporous (H-3DOM) structure. The functional can be further employed as ideal precursor synthesis cobalt on oxygen/nitrogen-co-doped carbon composites H-3DOM structures, hydrophilic surface. structure improve external surface area maximize exposure sites. Moreover, oxygen-containing groups enhance wettability guarantee more electrochemically accessible aqueous electrolyte. Benefitting from these outstanding characteristics, H-3DOM-Co/ONC exhibits high electrocatalytic activity oxygen reduction reaction, superior its counterparts without hierarchically ordered functionalization.

Язык: Английский

Процитировано

110