Water enables mild oxidation of methane to methanol on gold single-atom catalysts DOI Creative Commons
Laihao Luo, Jie Luo, Hongliang Li

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Feb. 22, 2021

Abstract As a 100% atom-economy process, direct oxidation of methane into methanol remains as grand challenge due to the dilemma between activation and over-oxidation methanol. Here, we report that water enabled mild with >99% selectivity over Au single atoms on black phosphorus (Au 1 /BP) nanosheets under light irradiation. The mass activity /BP reached 113.5 μmol g catal −1 in pressured 33 bar mixed gas (CH 4 :O 2 = 10:1) at 90 °C irradiation (1.2 W), while energy was 43.4 kJ mol . Mechanistic studies revealed assisted O generate reactive hydroxyl groups •OH radicals Hydroxyl reacted form CH 3 * species, followed by via Considering recycling during whole can also regard catalyst.

Language: Английский

Toward the Decentralized Electrochemical Production of H2O2: A Focus on the Catalysis DOI
Sungeun Yang,

Arnau Verdaguer‐Casadevall,

Logi Arnarson

et al.

ACS Catalysis, Journal Year: 2018, Volume and Issue: 8(5), P. 4064 - 4081

Published: March 28, 2018

H2O2 is a valuable, environmentally friendly oxidizing agent with wide range of uses from the provision clean water to synthesis valuable chemicals. The on-site electrolytic production would bring chemical applications beyond its present reach. successful commercialization electrochemical requires cathode catalysts high activity, selectivity, and stability. In this Perspective, we highlight our current understanding factors that control performance. We review influence catalyst material, electrolyte, structure interface at mesoscopic scale. provide original theoretical data on role geometry active site activity selectivity. have also conducted series experiments (i) effect pH glassy carbon, pure metals, metal–mercury alloys, (ii) cell mass transport in liquid half-cells comparison membrane electrode assemblies.

Language: Английский

Citations

918
Hydrophobic zeolite modification for in situ peroxide formation in methane oxidation to methanol DOI Open Access
Zhu Jin, Liang Wang, Erik Zuidema

et al.

Science, Journal Year: 2020, Volume and Issue: 367(6474), P. 193 - 197

Published: Jan. 10, 2020

Confining peroxide to make methanol In principle, hydrogen would be an efficient oxidant for the conversion of methane under mild conditions. practice, however, it is currently too expensive produce ahead time this purpose. Jin et al. report a catalyst system that generates and concentrates immediate reaction with methane. A hydrophobically coated zeolite keeps close gold palladium active site, where incoming then selectively oxidized methanol. Science , issue p. 193

Language: Английский

Citations

621
In Situ/Operando Electrocatalyst Characterization by X-ray Absorption Spectroscopy DOI Creative Commons
Janis Timoshenko, Beatriz Roldán Cuenya

Chemical Reviews, Journal Year: 2020, Volume and Issue: 121(2), P. 882 - 961

Published: Sept. 28, 2020

During the last decades, X-ray absorption spectroscopy (XAS) has become an indispensable method for probing structure and composition of heterogeneous catalysts, revealing nature active sites establishing links between structural motifs in a catalyst, local electronic structure, catalytic properties. Here we discuss fundamental principles XAS describe progress instrumentation data analysis approaches undertaken deciphering near edge (XANES) extended fine (EXAFS) spectra. Recent usages field catalysis, with emphasis on examples concerning electrocatalysis, will be presented. The latter is rapidly developing immense industrial applications but also unique challenges terms experimental characterization restrictions advanced modeling required. This review highlight new insight that can gained complex real-world electrocatalysts including their working mechanisms dynamic processes taking place course chemical reaction. More specifically, situ operando to probe catalyst’s interactions environment (support, electrolyte, ligands, adsorbates, reaction products, intermediates) its structural, chemical, transformations as it adapts conditions.

Language: Английский

Citations

556
Highly selective oxidation of methane to methanol at ambient conditions by titanium dioxide-supported iron species DOI
Jijia Xie, Renxi Jin, Ang Li

et al.

Nature Catalysis, Journal Year: 2018, Volume and Issue: 1(11), P. 889 - 896

Published: Oct. 29, 2018

Language: Английский

Citations

497
Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis DOI Creative Commons
Xianguang Meng,

Xiaoju Cui,

N. Pethan Rajan

et al.

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

Published: May 27, 2019

Language: Английский

Citations

456
Role of the Support in Gold-Containing Nanoparticles as Heterogeneous Catalysts DOI Creative Commons
Meenakshisundaram Sankar, Qian He, Rebecca V. Engel

et al.

Chemical Reviews, Journal Year: 2020, Volume and Issue: 120(8), P. 3890 - 3938

Published: March 30, 2020

In this review, we discuss selected examples from recent literature on the role of support directing nanostructures Au-based monometallic and bimetallic nanoparticles. The is then discussed in relation to catalytic properties nanoparticles using different gas phase liquid reactions. reactions include CO oxidation, aerobic oxidation monohydric polyhydric alcohols, selective hydrogenation alkynes, nitroaromatics, CO2 hydrogenation, C-C coupling, methane oxidation. Only studies where has been explicitly studied detail have for discussion. However, also examined involving unsupported metal (i.e., colloidal nanoparticles). It clear that functionality can play a crucial tuning activity observed advanced theory characterization add greatly our understanding these fascinating catalysts.

Language: Английский

Citations

376
Theory-oriented screening and discovery of advanced energy transformation materials in electrocatalysis DOI Creative Commons
Hongyu Jing, Peng Zhu, Xiaobo Zheng

et al.

Advanced Powder Materials, Journal Year: 2021, Volume and Issue: 1(1), P. 100013 - 100013

Published: Nov. 15, 2021

Various metal-based electrocatalysts from nanocrystals, to clusters and single-atoms, have been well-discovered towards high-efficient power devices electrocatalytic conversion. To accelerate energy transformation materials discovery, developing high-throughput DFT calculations machine-learning techniques is of great necessity. This review comprehensively outlines the latest progress theory-guided design advanced materials. Especially, we focus on study single atoms in various devices, such as fuel cell (oxygen reduction reaction, ORR; acid oxidation reaction; alcohol reaction), other reactions for energy-related conversion small molecules, H2O2 evolution (2e− ORR), water splitting (H2 reaction/O2 HER/OER), N2 reaction (NRR), CO2 (CO2RR). Firstly, electronic structure, interaction mechanism, activation path are discussed provide an overall blueprint electrocatalysis batteries mentioned above. Thereafter, experimental synthesis strategies, structural recognition, performance figured out. Finally, some viewpoints into current issues future concept provided.

Language: Английский

Citations

376
Metal-organic framework-based heterogeneous catalysts for the conversion of C1 chemistry: CO, CO2 and CH4 DOI
Wen‐Gang Cui, Guoying Zhang, Tong‐Liang Hu

et al.

Coordination Chemistry Reviews, Journal Year: 2019, Volume and Issue: 387, P. 79 - 120

Published: Feb. 19, 2019

Language: Английский

Citations

354
From Solar Energy to Fuels: Recent Advances in Light‐Driven C1 Chemistry DOI
Guangbo Chen, Geoffrey I. N. Waterhouse, Run Shi

et al.

Angewandte Chemie International Edition, Journal Year: 2019, Volume and Issue: 58(49), P. 17528 - 17551

Published: March 2, 2019

Abstract Catalytic C 1 chemistry based on the activation/conversion of synthesis gas (CO+H 2 ), methane, carbon dioxide, and methanol offers great potential for sustainable development hydrocarbon fuels to replace oil, coal, natural gas. Traditional thermal catalytic processes used transformations require high temperatures pressures, thereby carrying a significant footprint. In comparison, solar‐driven catalysis greener more pathway manufacturing other commodity chemicals, although conversion efficiencies are currently too low justify industry investment. this Review, we highlight recent advances milestones in light‐driven chemistry, including solar Fischer–Tropsch synthesis, water‐gas‐shift reaction, CO hydrogenation, as well methane reactions. Particular emphasis is placed rational design catalysts, structure–reactivity relationships, reaction mechanisms. Strategies scaling up also discussed.

Language: Английский

Citations

348
Direct and Selective Photocatalytic Oxidation of CH4 to Oxygenates with O2 on Cocatalysts/ZnO at Room Temperature in Water DOI
Hui Song, Xianguang Meng, Shengyao Wang

et al.

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

Citations

343