Chemical Synthesis of Single Atomic Site Catalysts

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11900 - 11955

Published: April 3, 2020

Manipulating metal atoms in a controllable way for the synthesis of materials with desired structure and properties is holy grail chemical synthesis. The recent emergence single atomic site catalysts (SASC) demonstrates that we are moving toward this goal. Owing to maximum efficiency atom-utilization unique structures properties, SASC have attracted extensive research attention interest. prerequisite scientific practical applications fabricate highly reactive stable on appropriate supports. In review, various synthetic strategies summarized concrete examples highlighting key issues methods stabilize supports suppress their migration agglomeration. Next, discuss how conditions affect catalytic before ending review by prospects challenges as well further researches SASC.

Language: Английский

---

Single-Atom Catalysts across the Periodic Table

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11703 - 11809

Published: Oct. 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.

Language: Английский

---

Direct transformation of bulk copper into copper single sites via emitting and trapping of atoms

Nature Catalysis, Journal Year: 2018, Volume and Issue: 1(10), P. 781 - 786

Published: Sept. 25, 2018

Language: Английский

---

Single-Atom Catalysts Based on the Metal–Oxide Interaction

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(21), P. 11986 - 12043

Published: Oct. 28, 2020

Metal atoms dispersed on the oxide supports constitute a large category of single-atom catalysts. In this review, supported catalysts are discussed about their synthetic procedures, characterizations, and reaction mechanism in thermocatalysis, such as water-gas shift reaction, selective oxidation/hydrogenation, coupling reactions. Some typical materials, including ferric oxide, cerium titanium dioxide, aluminum so on, intentionally mentioned for unique roles anchoring metal taking part catalytic The interactions between summarized to give picture how stabilize atomic centers, rationally tune geometric structures electronic states single atoms. Furthermore, several directions fabricating with improved performance proposed basis state-of-the-art understanding metal-oxide interactions.

Language: Английский

---

Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis

Chem, Journal Year: 2019, Volume and Issue: 5(9), P. 2296 - 2325

Published: May 27, 2019

Language: Английский

---

Theoretical insights into single-atom catalysts

Chemical Society Reviews, Journal Year: 2020, Volume and Issue: 49(22), P. 8156 - 8178

Published: Jan. 1, 2020

Single-atom catalysts (SACs) with atomically dispersed metals have emerged as a new class of heterogeneous and attracted considerable interest because they offer 100% metal atom utilization show excellent catalytic behavior compared traditionally supported nano-particles. However, it is challenging to explore the active sites mechanisms SACs through common characterization methods due isolated single atoms. Therefore, employing theoretical calculations determine nature SACs' reaction particularly meaningful. This paper describes by summarizing diverse applications properties SACs, which starts from computational simulation on couple important SACs. Then distinctive fundamental are discussed. At last, challenges future perspectives for outlined.

Language: Английский

---

Direct and Selective Photocatalytic Oxidation of CH₄ to Oxygenates with O₂ on Cocatalysts/ZnO at Room Temperature in Water

Journal of the American Chemical Society, Journal Year: 2019, Volume and Issue: 141(51), P. 20507 - 20515

Published: Dec. 13, 2019

Direct conversion of methane into methanol and other liquid oxygenates still confronts considerable challenges in activating the first C-H bond inhibiting overoxidation. Here, we report that ZnO loaded with appropriate cocatalysts (Pt, Pd, Au, or Ag) enables direct oxidation to formaldehyde water using only molecular oxygen as oxidant under mild light irradiation at room temperature. Up 250 micromoles ∼95% selectivity is achieved for 2 h over 10 mg 0.1 wt % Au. Experiments isotopically labeled reveal O2, rather than water, source CH4 oxidation. We find cocatalyst could concertedly activate O2 methyl radical mildly oxidative intermediate (hydroperoxyl radical) which are two key precursor intermediates generating oxygenated products Our study underlines equally significant aspects realizing selective photooxidation oxygenates, i.e., efficient activation controllable O2.

Language: Английский

---

Solar-Energy-Mediated Methane Conversion

Joule, Journal Year: 2019, Volume and Issue: 3(7), P. 1606 - 1636

Published: July 1, 2019

Language: Английский

---

Highly durable metal ensemble catalysts with full dispersion for automotive applications beyond single-atom catalysts

Nature Catalysis, Journal Year: 2020, Volume and Issue: 3(4), P. 368 - 375

Published: Feb. 17, 2020

Language: Английский

---

Directly transforming copper (I) oxide bulk into isolated single-atom copper sites catalyst through gas-transport approach

Nature Communications, Journal Year: 2019, Volume and Issue: 10(1)

Published: Aug. 19, 2019

Abstract Single-atom metal catalysts have sparked tremendous attention, but direct transformation of cheap and easily obtainable bulk oxide into single atoms is still a great challenge. Here we report facile versatile gas-transport strategy to synthesize isolated single-atom copper sites (Cu ISAS/NC) catalyst at gram levels. Commercial (I) powder sublimated as mobile vapor nearly melting temperature (1500 K) subsequently can be trapped reduced by the defect-rich nitrogen-doped carbon (NC), forming catalyst. Strikingly, this thermally stable Cu ISAS/NC, which obtained above 1270 K, delivers excellent oxygen reduction performance possessing recorded half-wave potential 0.92 V vs RHE among other Cu-based electrocatalysts. By varying precursors, demonstrate universal synthesis different anchored on NC materials (M where M refers Mo Sn). This readily scalable as-prepared sintering-resistant ISAS/NC hold in high-temperature applications.

Language: Английский

---