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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Cobalt single atom site catalysts with ultrahigh metal loading for enhanced aerobic oxidation of ethylbenzene

Nano Research, Год журнала: 2021, Номер 14(7), С. 2418 - 2423

Опубликована: Янв. 5, 2021

Язык: Английский

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Rational Design of Single‐Atom Site Electrocatalysts: From Theoretical Understandings to Practical Applications

Advanced Materials, Год журнала: 2021, Номер 33(34)

Опубликована: Июль 8, 2021

Atomically dispersed metal-based electrocatalysts have attracted increasing attention due to their nearly 100% atomic utilization and excellent catalytic performance. However, current fundamental comprehension summaries reveal the underlying relationship between single-atom site (SACs) corresponding application are rarely reported. Herein, understandings intrinsic mechanisms SACs electrocatalytic applications systemically summarized. Different preparation strategies presented synthetic with engineering well-defined on basis of theoretical principle (size effect, metal-support interactions, electronic structure coordination environment effect). Then, an overview is presented, including oxygen reduction reaction, hydrogen evolution oxidation small organic molecules, carbon dioxide nitrogen reaction. The structure-performance reactions also discussed in depth expound enhancement mechanisms. Finally, a summary provided perspective supplied demonstrate challenges opportunities for rational designing, synthesizing, modulating advanced toward reactions.

Язык: Английский

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Non-carbon-supported single-atom site catalysts for electrocatalysis

Energy & Environmental Science, Год журнала: 2021, Номер 14(5), С. 2809 - 2858

Опубликована: Янв. 1, 2021

Non-carbon supported SACs were classified into eight categories based on the nature of their substrates for first time, and corresponding anchoring stabilization mechanisms have been systematically summarized discussed.

Язык: Английский

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Engineering Bismuth–Tin Interface in Bimetallic Aerogel with a 3D Porous Structure for Highly Selective Electrocatalytic CO₂ Reduction to HCOOH

Angewandte Chemie International Edition, Год журнала: 2021, Номер 60(22), С. 12554 - 12559

Опубликована: Март 15, 2021

Abstract Electrochemical reduction of CO 2 (CO RR) into valuable hydrocarbons is appealing in alleviating the excessive level. We present very first utilization metallic bismuth–tin (Bi‐Sn) aerogel for RR with selective HCOOH production. A non‐precious bimetallic Bi‐Sn readily prepared at ambient temperature, which exhibits 3D morphology interconnected channels, abundant interfaces and a hydrophilic surface. Superior to Bi Sn, exposes more active sites it has favorable mass transfer properties, endow high FE 93.9 %. Moreover, achieves ca. 90 % that was maintained 10 h flow battery. In situ ATR‐FTIR measurements confirmed formation *HCOO rate‐determining step toward formic acid generation. DFT demonstrated coexistence Sn optimized energy barrier production HCOOH, thereby improving catalytic activity.

Язык: Английский

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Synergistic Effect of Atomically Dispersed Ni–Zn Pair Sites for Enhanced CO₂ Electroreduction

Advanced Materials, Год журнала: 2021, Номер 33(41)

Опубликована: Авг. 31, 2021

Abstract Dual‐atom catalysts have the potential to outperform well‐established single‐atom for electrochemical conversion of CO 2 . However, lack understanding regarding mechanism this enhanced catalytic process prevents rational design high‐performance catalysts. Herein, an obvious synergistic effect in atomically dispersed Ni–Zn bimetal sites is observed. In situ characterization combined with density functional theory (DFT) calculations reveals that heteronuclear coordination modifies d‐states metal atom, narrowing gap between d‐band centre (ε d ) Ni (3d) orbitals and Fermi energy level ( E F strengthen electronic interaction at reaction interface, resulting a lower free barrier (Δ G thermodynamic pathway reduced activation as well fortified metal–C bonding kinetic pathway. Consequently, faradaic efficiency >90% obtained across broad window from − 0.5 1.0 V (vs RHE), reaching maximum 99% −0.8 V, superior Ni/Zn single‐metal sites.

Язык: Английский

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P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO₂Reduction to Hydrocarbon Fuels with High C₂H₆Evolution

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(40)

Опубликована: Авг. 15, 2022

The light-driven CO2 reduction to multi-carbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish C-C coupling greatly hinder its development. Herein, we report a photocatalyst comprising P Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves high C2 H6 evolution rate 616.6 μmol g-1 h-1 in reducing hydrocarbons. detailed spectroscopic characterizations identify formation charge-enriched sites, where isolated atoms serve as hole capture during photocatalysis. Theoretical simulations combined with situ FTIR measurement reveal kinetically feasible process for intermediate (*OC-COH) confirm favorable production P/Cu SAs@CN photocatalyst. This work offers new insights into design atomic precision toward highly efficient photocatalytic conversion value-added products.

Язык: Английский

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Engineering the Local Atomic Environments of Indium Single‐Atom Catalysts for Efficient Electrochemical Production of Hydrogen Peroxide

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(12)

Опубликована: Янв. 19, 2022

The in-depth understanding of local atomic environment-property relationships p-block metal single-atom catalysts toward the 2 e- oxygen reduction reaction (ORR) has rarely been reported. Here, guided by first-principles calculations, we develop a heteroatom-modified In-based metal-organic framework-assisted approach to accurately synthesize an optimal catalyst, in which single In atoms are anchored combined N,S-dual first coordination and B second supported hollow carbon rods (In SAs/NSBC). SAs/NSBC catalyst exhibits high H2 O2 selectivity above 95 % wide range pH. Furthermore, SAs/NSBC-modified natural air diffusion electrode unprecedented production rate 6.49 mol peroxide gcatalyst-1 h-1 0.1 M KOH electrolyte 6.71 PBS electrolyte. This strategy enables design next-generation high-performance materials, provides practical guidance for electrosynthesis.

Язык: Английский

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Single‐atom catalysis for carbon neutrality

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

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Heterogeneous catalysts for CO₂hydrogenation to formic acid/formate: from nanoscale to single atom

Energy & Environmental Science, Год журнала: 2021, Номер 14(3), С. 1247 - 1285

Опубликована: Янв. 1, 2021

This review provides an overview of advances on constructing heterogeneous nanostructured and single atom catalysts for CO₂hydrogenation to formic acid/formate. The main focus is placed structure–activity correlations mechanistic insights.

Язык: Английский

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