Surface Density Dependent Catalytic Activity of Single Palladium Atoms Supported on Ceria** DOI
Yongseon Kim, Greg Collinge, Mal‐Soon Lee

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(42), P. 22769 - 22775

Published: June 28, 2021

Abstract The analogy between single‐atom catalysts (SACs) and molecular predicts that the specific catalytic activity of these systems is constant. We provide evidence this prediction not necessarily true. As a case in point, we show over ceria‐supported single Pd atoms linearly increases with metal atom density, originating from cumulative enhancement CeO 2 reducibility. long‐range electrostatic footprints (≈1.5 nm) around each site overlap other as surface density increases, resulting an observed deviation constant activity. These cooperative effects exhaust previously active O above certain leading to their permanent removal consequent drop reaction rate. findings our combined experimental computational study reducible oxide‐supported can be tuned by varying atoms.

Language: Английский

Interlayer Charge Transfer Regulates Single-Atom Catalytic Activity on Electride/Graphene 2D Heterojunctions DOI
Wei Li, Cong Liu,

Chenkai Gu

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(8), P. 4774 - 4783

Published: Feb. 17, 2023

Single-atom catalysts with structure and activity tunability have attracted significant attention for energy environmental applications. Herein we present a first-principles study of single-atom catalysis on two-dimensional graphene electride heterostructures. The anion electron gas in the layer enables colossal transfer to layer, degree being controllable by selection electride. charge tunes d-orbital occupancy single metal atom, enhancing catalytic hydrogen evolution reactions oxygen reduction reactions. strong correlation between adsorption Eads variation Δq suggests that interfacial is critical descriptor heterostructure-based catalysts. polynomial regression model proves importance accurately predicts ions molecules. This provides strategy obtain high-efficiency using

Language: Английский

Citations

84
Exploring the properties, types, and performance of atomic site catalysts in electrochemical hydrogen evolution reactions DOI Creative Commons
M. Nur Hossain, Lei Zhang, Roberto Neagu

et al.

Chemical Society Reviews, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 1, 2025

This review investigates atomic site catalysts (ASCs) for electrochemical hydrogen evolution reaction (HER), discussing their properties, types, performance, significance, activity, selectivity, stability, challenges, and future research directions.

Language: Английский

Citations

2
Single-atom catalysts for CO oxidation, CO2 reduction, and O2 electrochemistry DOI
Wenyu Yuan, Yiyuan Ma, Heng Wu

et al.

Journal of Energy Chemistry, Journal Year: 2021, Volume and Issue: 65, P. 254 - 279

Published: June 5, 2021

Language: Английский

Citations

70
Perspectives on Multifunctional Catalysts Derived from Layered Double Hydroxides toward Upgrading Reactions of Biomass Resources DOI
Yusen Yang,

Zhen Ren,

Shijie Zhou

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(11), P. 6440 - 6454

Published: May 17, 2021

Heterogeneous upgrading reactions serve as a promising and pivotal strategy for efficient utilization of biomass resources chemical energy, fuel, hydrogen, in which supported catalysts play key role determining catalytic activity selectivity desirable products. Biomass is the only renewable organic carbon resource nature, its conversion (e.g., hydrogenation, hydrodeoxygenation, oxidation, alkylation, halogenation, or nitration) to variety intermediates feedstocks has attracted increasing attention fundamental investigations industrial productions. The efficiency heterogeneous above highly rests with properties metals, supports, additives, well reactors reaction conditions (solvent, pressure, temperature). Recently, multifunctional derived from layered double hydroxides (LDHs) precursors have displayed outstanding performance, made great contribution development on high-value resources. elaborate regulation surface interface structure, geometric electronic defect coordination structure via tuning composition, structural architecture, topotactic transformation process LDHs imposes significant influence resulting behavior. Moreover, detailed structure–property relationship by virtue comprehensive studies provide innovative strategies synthesis high-efficiency LDHs-derived characteristics. In this Perspective, basis achievement representative studies, we put forward some suggestions prospects future.

Language: Английский

Citations

66
Complete CO Oxidation by O2 and H2O over Pt–CeO2−δ/MgO Following Langmuir–Hinshelwood and Mars–van Krevelen Mechanisms, Respectively DOI
Yanru Wang,

Jiamin Ma,

Xiuyi Wang

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(19), P. 11820 - 11830

Published: Sept. 9, 2021

CO oxidation has attracted great attention in the automobile exhaust treatment and fuel cell industrial process, with Pt as one of most promising catalysts. The efficiency catalyst is still below requirement industry due to limited understanding about reaction mechanism by O2 or H2O, which were proposed be following similar/same (the Mars–van Krevelen mechanism). Our recent results indicate that this assumption might not correct. Here, we design a combination isolated platinum atoms (Pt1) nanoparticles (Ptn) supported on MgO-dispersed CeO2−δ (CeO2−δ/MgO), named 0.5Pt–xCeO2−δ/MgO (x = 0, 1, 2, 5, 10, 20) establish two types active sites, solely over NPs (type-I) other at interface between reducible metal oxide support (type-II), perform kinetic, thermodynamic, situ spectroscopy analysis prove undergoes Langmuir–Hinshelwood type-I sites (Pt NPs), while water–gas shift (WGS) (type-II) verified activation energy assessment reactant product pressure dependency studies applied, systematic reduction barrier (by O2) was obtained once size increased independent changes CeO2−δ, WGS very sensitive slightly inert against NPs. Additionally, there competitive adsorption Pt–CeO2−δ/MgO, no H2O based our studies. Collectively, current work provides convincing evidence promotion change rather than simple effect hydroxyl dissociated dosing.

Language: Английский

Citations

64
Techniques for the characterization of single atom catalysts DOI Creative Commons
Ping Qi, Jian Wang,

Xavier Djitcheu

et al.

RSC Advances, Journal Year: 2022, Volume and Issue: 12(2), P. 1216 - 1227

Published: Jan. 1, 2022

In this paper, eight methods for identifying single atom catalysts are reviewed. Two of them can directly observe the existence atoms, while other provide corresponding evidence atoms.

Language: Английский

Citations

61
Toward Rational Design of Dual-Metal-Site Catalysts: Catalytic Descriptor Exploration DOI
Chuanyi Jia, Qian Wang, Jing Yang

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(6), P. 3420 - 3429

Published: March 1, 2022

Dual-metal-site catalysts (DMSCs) have emerged as a frontier in heterogeneous catalysis, while the underlying relationships connecting their dual-site synergistic effects on catalytic performance remain unclear. Here we present comprehensive first-principles study of O2 activation and CO oxidation series N-coordinated DMSCs. We discovered that N3-coordinated-adjacent dual-metal model has stronger dynamic effects, leading to much higher activity than others investigated. Based this model, detailed comparisons various metal combinations (M = Fe, Co, Ni, Cu, Pt) show Fe-containing are generally more active others. In particular, Fe–Ni combination, owing its preferential coadsorption CO+O2 highest is identified most promising candidate for oxidation. To explore some universal descriptors different combinations, (50 total) were systemically studied. It found designed electronic/spectral charge transfer, average metals, d-orbital center stretching vibrational frequency reactants may reflect binding ability/stability lone reactant. However, multiple (CO+O2), stability/reactivity key-species (O2) descriptor better performance. The transferability such multimolecular catalysis was confirmed by applying them NO These novel highlight importance structure–activity under reaction conditions, thus providing potential design strategies high-efficiency

Language: Английский

Citations

59
Rhodium Single‐Atom Catalyst Design through Oxide Support Modulation for Selective Gas‐Phase Ethylene Hydroformylation DOI Creative Commons
Marcos G. Farpón, Wilson Henao,

Philipp N. Pleßow

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(1)

Published: Oct. 31, 2022

A frontier challenge in single-atom (SA) catalysis is the design of fully inorganic sites capable emulating high reaction selectivity traditionally exclusive organometallic counterparts homogeneous catalysis. Modulating direct coordination environment SA sites, via exploitation oxide support's surface chemistry, stands as a powerful albeit underexplored strategy. We report that isolated Rh atoms stabilized on oxygen-defective SnO2 uniquely unite excellent TOF with essentially full gas-phase hydroformylation ethylene, inhibiting thermodynamically favored olefin hydrogenation. Density Functional Theory calculations and characterization suggest substantial depletion catalyst lattice oxygen, energetically facile , key to unlock pliability at mononuclear centers, leading an exceptional performance which par molecular catalysts liquid media.

Language: Английский

Citations

52
Anchoring single Ni atoms on CeO2 nanospheres as an efficient catalyst for the hydrogenolysis of lignin to aromatic monomers DOI
Ming Jiang, Xiaopeng Chen, Linlin Wang

et al.

Fuel, Journal Year: 2022, Volume and Issue: 324, P. 124499 - 124499

Published: May 10, 2022

Language: Английский

Citations

39
Transition Metal Single Atoms Constructed by Using Inherent Confined Space DOI

Meng‐Xuan Gu,

Le-Ping Gao,

Song‐Song Peng

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(5), P. 5025 - 5032

Published: Feb. 24, 2023

Single-atom catalysts (SACs) show expressively enhanced activity toward diverse reactions due to maximized atomic utilization of metal sites, while their facile, universal, and massive preparation remains a pronounced challenge. Here we report facile strategy for the SACs by use inherent confined space between template silica walls in template-occupied mesoporous SBA-15 (TOS). Different transition precursors can be introduced into readily grinding, during succeeding calcination single atoms are constructed form M–O–Si (M = Cu, Co, Ni, Zn). In addition generality, present is easy scale up allow synthesis 10 g one pot through ball milling. The Cu SAC has been applied CO2 cycloaddition epichlorohydrin, obviously higher than counterpart prepared without various reported Cu-containing catalysts.

Language: Английский

Citations

31