Atomically Dispersed Co-N/C Catalyst for Divergent Synthesis of Nitrogen-Containing Compounds from Alkenes DOI
Wenxuan Xue, Zhiwei Zhu,

Sanxia Chen

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(7), P. 4142 - 4149

Published: Feb. 8, 2023

Alkene functionalization with a single-atom catalyst (SAC) which merges homogeneous and heterogeneous catalysis is fascinating route to obtain high-value-added molecules. However, C–N bond formation of alkene SAC still unexplored. Herein, bimetal-organic framework-derived Co–N/C an atomically dispersed cobalt center reported show good activity chemoselective aziridination/oxyamination reactions from hydroxylamine, late-stage complex alkenes diversified synthetic transformations the aziridine product further expand utility this method. Moreover, system proceeds without external oxidants exhibits mild, atom-economic, recyclable characters. Detailed spectroscopic characterizations mechanistic studies revealed structure catalytic possible intermediates involved in mechanism cycle.

Language: Английский

The role of Cu1–O3 species in single-atom Cu/ZrO2 catalyst for CO2 hydrogenation DOI

Huibo Zhao,

Ruofan Yu,

Sicong Ma

et al.

Nature Catalysis, Journal Year: 2022, Volume and Issue: 5(9), P. 818 - 831

Published: Sept. 15, 2022

Language: Английский

Citations

378
Noble-metal single-atoms in thermocatalysis, electrocatalysis, and photocatalysis DOI

Fei-Fei Zhang,

Yinlong Zhu, Qian Lin

et al.

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(5), P. 2954 - 3009

Published: Jan. 1, 2021

This review summarizes the recent advances about noble-metal single-atom catalysts in thermocatalysis, electrocatalysis, and photocatalysis.

Language: Английский

Citations

288
Towards the development of the emerging process of CO2heterogenous hydrogenation into high-value unsaturated heavy hydrocarbons DOI
Jian Wei,

Ruwei Yao,

Yu Han

et al.

Chemical Society Reviews, Journal Year: 2021, Volume and Issue: 50(19), P. 10764 - 10805

Published: Jan. 1, 2021

This review covers recent developments in the synthesis of α-olefins and aromatics from CO 2 hydrogenation via direct indirect routes.

Language: Английский

Citations

254
Role of oxygen vacancy in metal oxides for photocatalytic CO2 reduction DOI
Wenbin Jiang,

Hongyi Loh,

Beverly Qian Ling Low

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 122079 - 122079

Published: Oct. 17, 2022

Language: Английский

Citations

226
Coordination tailoring of Cu single sites on C3N4 realizes selective CO2 hydrogenation at low temperature DOI Creative Commons
Yang Tang,

Xinnan Mao,

Ying Zhang

et al.

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

Published: Oct. 15, 2021

CO2 hydrogenation has attracted great attention, yet the quest for highly-efficient catalysts is driven by current disadvantages of poor activity, low selectivity, and ambiguous structure-performance relationship. We demonstrate here that C3N4-supported Cu single atom with tailored coordination structures, namely, Cu-N4 Cu-N3, can serve as highly selective active at temperature. The modulation structure readily realized simply altering treatment parameters. Further investigations reveal favors to form CH3OH via formate pathway, while Cu-N3 tends catalyze produce CO reverse water-gas-shift (RWGS) pathway. Significantly, productivity selectivity reach 4.2 mmol g-1 h-1 95.5%, respectively, catalyst. anticipate this work will promote fundamental researches on relationship catalysts.

Language: Английский

Citations

219
Highly Active Ir/In2O3 Catalysts for Selective Hydrogenation of CO2 to Methanol: Experimental and Theoretical Studies DOI
Chenyang Shen, Kaihang Sun, Zhitao Zhang

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(7), P. 4036 - 4046

Published: March 17, 2021

Iridium (Ir) catalysts have been extensively applied in homogeneous and photocatalytic CO2 conversion. However, hydrogenation to methanol over the supported Ir catalyst a heterogeneous flowing reactor has not reported yet. Here, we report that indium oxide (Ir/In2O3) of high dispersion is very active for methanol. Compared In2O3, Ir/In2O3 shows significantly higher activity with even selectivity. For example, conversion 17.7% achieved on 10 wt % loading selectivity 70% space time yield 0.765 gMeOH h–1 gcat–1 at 4/1 CO2/H2 feed ratio, 21 000 h–1, 300 °C, 5 MPa. With tested, causes activity. The characterization confirms an intense interaction between iridium which Ir–In2O3 interface as site selective into only enhances formation oxygen vacancies but also stabilizes improved activation. Further density functional theory studies reveal reverse water–gas shift route more favorable formate catalyst.

Language: Английский

Citations

174
Toward efficient single-atom catalysts for renewable fuels and chemicals production from biomass and CO2 DOI Creative Commons
Yubing Lu, Zihao Zhang, Huamin Wang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 292, P. 120162 - 120162

Published: March 20, 2021

Language: Английский

Citations

165
Recent advances of single-atom catalysts in CO2conversion DOI

Shunwu Wang,

Ligang Wang, Dingsheng Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(7), P. 2759 - 2803

Published: Jan. 1, 2023

The catalytic transformation of CO 2 into valuable fuels/chemicals is a promising and economically profitable process because it offers an alternative toward fossil feedstocks the benefit transforming cycling on scale-up.

Language: Английский

Citations

142
Highly Efficient CO2 Electroreduction to Methanol through Atomically Dispersed Sn Coupled with Defective CuO Catalysts DOI
Weiwei Guo, Shoujie Liu,

Xingxing Tan

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(40), P. 21979 - 21987

Published: Aug. 4, 2021

Abstract Using renewable electricity to drive CO 2 electroreduction is an attractive way achieve carbon‐neutral energy cycle and produce value‐added chemicals fuels. As important platform molecule clean fuel, methanol requires 6‐electron transfer in the process of reduction. Currently, suffers from poor efficiency low selectivity. Herein, we report first work design atomically dispersed Sn site anchored on defective CuO catalysts for methanol. It exhibits high Faradaic (FE) 88.6 % with a current density 67.0 mA cm −2 remarkable stability H‐cell, which highest FE(methanol) such compared results reported date. The atomic site, adjacent oxygen vacancy support cooperate very well, leading higher double‐layer capacitance, larger adsorption capacity lower interfacial charge resistance. Operando experiments functional theory calculations demonstrate that catalyst beneficial activation via decreasing barrier *COOH dissociation form *CO. obtained key intermediate *CO then bound Cu species further reduction, selectivity toward

Language: Английский

Citations

141
Ti‐doped CeO2 Stabilized Single‐Atom Rhodium Catalyst for Selective and Stable CO2 Hydrogenation to Ethanol DOI
Ke Zheng, Yufeng Li, Bing Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(44)

Published: Sept. 9, 2022

Development of effective and stable catalysts for CO2 hydrogenation into ethanol remains a challenge. Herein, we report that Rh1 /CeTiOx single-atom catalyst constructed by embedding monoatomic Rh onto Ti-doped CeO2 support has shown super high selectivity (≈99.1 %), record-breaking turnover frequency (493.1 h-1 ), outstanding stability. Synergistic effects Ti-doption contribute to this excellent catalytic performance firstly facilitating oxygen vacancies formation generate oxygen-vacancy-Rh Lewis-acid-base pairs, which favor adsorption activation, cleavage C-O bonds in CHx OH* COOH* * CO* species, subsequent C-C coupling ethanol, secondly generating strong Rh-O bond Ti-doping-induced crystal reconstruction, contributes striking This work highlights the importance elaborating regulation design substantially improve performance.

Language: Английский

Citations

136