Single-Atom Catalysts across the Periodic Table

Chemical Reviews, Год журнала: 2020, Номер 120(21), С. 11703 - 11809

Опубликована: Окт. 21, 2020

Isolated atoms featuring unique reactivity are at the heart of enzymatic and homogeneous catalysts. In contrast, although concept has long existed, single-atom heterogeneous catalysts (SACs) have only recently gained prominence. Host materials similar functions to ligands in catalysts, determining stability, local environment, electronic properties isolated thus providing a platform for tailoring targeted applications. Within just decade, we witnessed many examples SACs both disrupting diverse fields catalysis with their distinctive substantially enriching our understanding molecular processes on surfaces. To date, term SAC mostly refers late transition metal-based systems, but numerous exist which other elements play key catalytic roles. This review provides compositional encyclopedia SACs, celebrating 10th anniversary introduction this term. By defining broadest sense, explore full elemental diversity, joining different areas across whole periodic table, discussing historical milestones recent developments. particular, examine coordination structures associated accessed through distinct single-atom–host combinations relate them main applications thermo-, electro-, photocatalysis, revealing trends element-specific evolution, host design, uses. Finally, highlight frontiers field, including multimetallic atom proximity control, possible multistep cascade reactions, identifying challenges, propose directions future development flourishing field.

Язык: Английский

---

Single-atom catalysis in advanced oxidation processes for environmental remediation

Chemical Society Reviews, Год журнала: 2021, Номер 50(8), С. 5281 - 5322

Опубликована: Янв. 1, 2021

This review presents the recent advances in synthetic strategies, characterisation, and computations of carbon-based single-atom catalysts, as well their innovative applications mechanisms advanced oxidation technologies.

Язык: Английский

---

Modulating the local coordination environment of single-atom catalysts for enhanced catalytic performance

Nano Research, Год журнала: 2020, Номер 13(7), С. 1842 - 1855

Опубликована: Март 30, 2020

Язык: Английский

---

High temperature proton exchange membrane fuel cells: progress in advanced materials and key technologies

Chemical Society Reviews, Год журнала: 2020, Номер 50(2), С. 1138 - 1187

Опубликована: Ноя. 27, 2020

This comprehensive review gives a picture about the state-of-the-art progress of HT-PEMFCs, and challenges, strategies rules to design, evaluate promote performance HT-PEMFCs.

Язык: Английский

---

Coexisting Single‐Atomic Fe and Ni Sites on Hierarchically Ordered Porous Carbon as a Highly Efficient ORR Electrocatalyst

Advanced Materials, Год журнала: 2020, Номер 32(42)

Опубликована: Сен. 16, 2020

The development of oxygen reduction reaction (ORR) electrocatalysts based on earth-abundant nonprecious materials is critically important for sustainable large-scale applications fuel cells and metal-air batteries. Herein, a hetero-single-atom (h-SA) ORR electrocatalyst presented, which has atomically dispersed Fe Ni coanchored to microsized nitrogen-doped graphitic carbon support with unique trimodal-porous structure configured by highly ordered macropores interconnected through mesopores. Extended X-ray absorption fine spectra confirm that Fe- Ni-SAs are affixed the via FeN4 NiN4 coordination bonds. resultant Fe/Ni h-SA exhibits an outstanding activity, outperforming SA only or Ni-SAs, benchmark Pt/C. obtained experimental results indicate achieved performance from synergetic enhancement induced coexisting sites, superior mass-transfer capability promoted trimodal-porous-structured support.

Язык: Английский

---

Recent advances of noble-metal-free bifunctional oxygen reduction and evolution electrocatalysts

Chemical Society Reviews, Год журнала: 2021, Номер 50(13), С. 7745 - 7778

Опубликована: Янв. 1, 2021

Bifunctional oxygen reduction and evolution constitute the core processes for sustainable energy storage. The advances on noble-metal-free bifunctional electrocatalysts are reviewed.

Язык: Английский

---

Understanding the inter-site distance effect in single-atom catalysts for oxygen electroreduction

Nature Catalysis, Год журнала: 2021, Номер 4(7), С. 615 - 622

Опубликована: Июль 19, 2021

Язык: Английский

---

Recent Advances in MOF‐Derived Single Atom Catalysts for Electrochemical Applications

Advanced Energy Materials, Год журнала: 2020, Номер 10(38)

Опубликована: Авг. 13, 2020

Abstract Electrocatalysis plays a critical role in clean energy conversion, enabling great improvement for future sustainable technologies. Single atom catalysts (SACs) derived from metal–organic framework (MOF) are emerging extraordinary materials electrochemical catalytic applications. Covering the merits of unique electronic structure, low‐coordination environment, quantum size effect, and metal–support interaction, SACs promise enhanced electrocatalytic activity, stability, selectivity field conversion. In this article, MOF synthesis routes to afford well‐dispersed along with respective mechanism systematically reviewed first, typical examples each strategy carefully discussed. Then characterization techniques understanding isolated spatial distribution, local coordination environment SACs, insights into stable mechanisms provided by density functional theory (DFT) calculations summarized. addition, several important applications MOF‐derived including oxygen reduction reaction, CO 2 nitrogen hydrogen evolution etc., highlighted. To facilitate development high‐performing technical challenges corresponding research directions proposed.

Язык: Английский

---

Atomically Dispersed Co₂–N₆ and Fe–N₄ Costructures Boost Oxygen Reduction Reaction in Both Alkaline and Acidic Media

Advanced Materials, Год журнала: 2021, Номер 33(49)

Опубликована: Окт. 8, 2021

Abstract Polynary transition‐metal atom catalysts are promising to supersede platinum (Pt)‐based for oxygen reduction reaction (ORR). Regulating the local configuration of atomic is key catalyst performance enhancement. Different from previously reported single‐atom or dual‐atom configurations, a new type ternary‐atom catalyst, which consists atomically dispersed, nitrogen‐coordinated Co–Co dimers, and Fe single sites (i.e., Co 2 –N 6 Fe–N 4 structures) that coanchored on highly graphitized carbon supports developed. This unique ORR outperforms with only in both alkaline acid conditions. Density functional theory calculations clearly unravels synergistic effect sites, can induce higher filling degree Fe–d orbitals favors binding capability *OH intermediates (the rate determining step). may be alternative Pt drive cathodic zinc–air batteries.

Язык: Английский

---

Boosting Oxygen Electrocatalytic Activity of Fe–N–C Catalysts by Phosphorus Incorporation

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(6), С. 3647 - 3655

Опубликована: Фев. 6, 2023

Nitrogen-doped graphitic carbon materials hosting single-atom iron (Fe-N-C) are major non-precious metal catalysts for the oxygen reduction reaction (ORR). The nitrogen-coordinated Fe sites described as first coordination sphere. As opposed to good performance in ORR, that evolution (OER) is extremely poor due sluggish O-O coupling process, thus hampering practical applications of rechargeable zinc (Zn)-air batteries. Herein, we succeed boosting OER activity Fe-N-C by additionally incorporating phosphorus atoms into second sphere, here denoted P/Fe-N-C. resulting material exhibits excellent 0.1 M KOH with an overpotential low 304 mV at a current density 10 mA cm-2. Even more importantly, they exhibit remarkably small ORR/OER potential gap 0.63 V. Theoretical calculations using first-principles functional theory suggest enhances electrocatalytic balancing *OOH/*O adsorption FeN4 sites. When used air cathode Zn-air battery, P/Fe-N-C delivers charge-discharge high peak power 269 mW cm-2, highlighting its role state-of-the-art bifunctional electrocatalyst.

Язык: Английский

---