Adjacent single-atom irons boosting molecular oxygen activation on MnO2

Gu, Huayu; Liu, Xiao; Ling, Cancan; Wei, Kai; Zhan, Guangming; Guo, Yanbing; Zhang, Lizhi

doi:10.1038/s41467-021-25726-w

Cited by 129 publications

(108 citation statements)

References 45 publications

Supporting

Mentioning

105

Contrasting

Order By: Relevance

“…Oxygen gas is commonly recognized as the most atom-economical and environmentally benign oxidant for use in oxidation reactions. [6][7][8] Most studies are focused on noble or platinum-group metalbased catalysts toward this oxidation reaction. For example, To the best of our knowledge, very few studies have been focused on the non-noble metal-based single atom catalysts for aerobic oxidation of alcohols.…”

Section: Introductionmentioning

confidence: 99%

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Fan

et al. 2022

Small

View full text Add to dashboard Cite

Lee et al. reported a series of highly active single-site mesoporous Pd/Al 2 O 3 catalysts for selective aerobic oxidation of allylic alcohols. [9] Grassi et al. described gold nanoparticles enclosed in a polymer matrix for oxidative esterification of cinnamyl alcohol with alkyl alcohols. [10] Lee and co-workers developed a zirconia-supported ruthenium catalyst for efficient aerobic oxidation of alcohols to aldehydes. [11] Li et al. found that metal/oxide supported catalysts, such as FeO/Pt(111) or Cu 2 O/ Ag(111) exhibit interfacial effects that significantly improve the efficacy in the selective oxidation of primary alcohols. [4] These nanoparticle-based catalysts, though effective in mediating selective oxidation reactions, have significant drawbacks of high cost, low selectivity, and rapid deactivation in harsh conditions. As such, the development of more practical and economical catalyst systems has been a major challenge in both industrial and academic areas.In 2011, Zhang and co-workers, for the first time, presented a comprehensive study and coined the concept of single-atom catalysis. [12] As a new frontier, single atom catalysts (SACs) have gained wide attention because of their great advantages of high atom efficiency and unique catalytic activity. [13][14][15][16][17][18][19][20] SACs possess distinctive chemical and physical properties and a unique coordination environment that is different from their nanoparticle counterparts. [21][22][23][24][25] Moreover, SACs have been found to be effective in bridging homogeneous and heterogeneous catalysis. [26][27][28][29] Selective aerobic oxidation of alcohols offers an attractive means to address challenges in the modern chemical industry, but the development of nonnoble metal catalysts with superior efficacy for this reaction remains a grand challenge. Here, this study reports on such a catalyst based on atomically defined undercoordinated copper atoms over nitrogen-doped carbon support as an efficient, durable, and scalable heterogeneous catalyst for selective aerobic oxidation of alcohols. This catalyst exhibits extremely high intrinsic catalytic activity (TOF of 7692 h −1 ) in the oxidation of cinnamyl alcohol to afford cinnamaldehyde, along with exceptional recyclability (at least eight cycles), scalability, and broad substrate scope. DFT calculations suggest that the high activity derives from the low oxidation state and the unique co ordination environment of the copper sites in the catalyst. These findings pave the way for the design of highly active and stable single atom catalysts to potentially address challenges in synthetic chemistry.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/smll.202106614.

show abstract

Section: Introductionmentioning

confidence: 99%

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Fan

et al. 2022

Small

View full text Add to dashboard Cite

show abstract

“…Other than liquid biofuel and gas biofuel processes, SACs and SAAs have recently shown great promise for environmental catalysis against a variety of pollutants due to the maximum site exposure by SACs and SAAs. It should be noted that SACs and SAAs can also be used effectively for major reactions such as the electrochemical oxidation of volatile organic compounds (VOCs), dehydrogenation of VOCs, and SO 3 decomposition [160,161]. CN-0.2Ni-HO (CN: nitride) Photocatalytic water splitting Hydrogen -Photocatalytic H 2 production rate was the highest (354.9 µmol h −1 g −1 ), higher than that of reported CN photocatalysts SACs.…”

Section: The Challenge and Opportunities Of Sacs And Saas In Biofuel Productionmentioning

confidence: 94%

“…For instance, VOCs can be efficaciously oxidised into water, CO 2 , and additional nontoxic substances at low temperatures using catalytic oxidation. Thus, there is significant potential for the application of SAAs for diverse catalytic reactions in the environmental sector [86,161,164] 4.…”

mentioning

confidence: 99%

Single-Atom Catalysts: A Review of Synthesis Strategies and Their Potential for Biofuel Production

et al. 2021

View full text Add to dashboard Cite

Biofuels have been derived from various feedstocks by using thermochemical or biochemical procedures. In order to synthesise liquid and gas biofuel efficiently, single-atom catalysts (SACs) and single-atom alloys (SAAs) have been used in the reaction to promote it. SACs are made up of single metal atoms that are anchored or confined to a suitable support to keep them stable, while SAAs are materials generated by bi- and multi-metallic complexes, where one of these metals is atomically distributed in such a material. The structure of SACs and SAAs influences their catalytic performance. The challenge to practically using SACs in biofuel production is to design SACs and SAAs that are stable and able to operate efficiently during reaction. Hence, the present study reviews the system and configuration of SACs and SAAs, stabilisation strategies such as mutual metal support interaction and geometric coordination, and the synthesis strategies. This paper aims to provide useful and informative knowledge about the current synthesis strategies of SACs and SAAs for future development in the field of biofuel production.

show abstract

“…83,84 And through the least-squares tting of Fourier transform EXAFS (FT-EXAFS), accurate values about coordinate number and bond length can be obtained. 85,86 Besides, so XAS has unique advantages in investigating orbital hybridization between metal and light ligand elements by employing so X-ray as the excited light source. 87 Different from techniques focusing on supercial chemical environments like XPS, XAS implies total statistical results of catalyst bulks owing to superior penetration depth of X-ray, which makes visualizing operando and in situ variation of serving SACs possible (Fig.…”

Section: Xasmentioning

confidence: 99%

Synchrotron-radiation spectroscopic identification towards diverse local environments of single-atom catalysts

Qiao

Zhang

et al. 2022

J. Mater. Chem. A

View full text Add to dashboard Cite

show abstract

Adjacent single-atom irons boosting molecular oxygen activation on MnO2

Cited by 129 publications

References 45 publications

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Atomically Defined Undercoordinated Copper Active Sites over Nitrogen‐Doped Carbon for Aerobic Oxidation of Alcohols

Single-Atom Catalysts: A Review of Synthesis Strategies and Their Potential for Biofuel Production

Synchrotron-radiation spectroscopic identification towards diverse local environments of single-atom catalysts

Contact Info

Product

Resources

About