Covalent-bonding to irreducible SiO2 leads to high-loading and atomically dispersed metal catalysts

Zhu, Yulong; Kong, Xiao; Yin, Junqing; You, Rui; Zhang, Bin; Zheng, Hongyan; Wen, Xiaodong; Zhu, Yulei; Li, Yongwang

doi:10.1016/j.jcat.2017.07.030

Cited by 54 publications

(41 citation statements)

References 59 publications

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“…The chemical shift of the Cu 2p 3/2 level to higher binding energy implied a charge transfer from the metal ion toward the support oxide . That is, CuPSs, particularly 30CuPS, should have stronger Cu‐SiO 2 interactions than that of Cu/SiO 2 …”

Section: Resultsmentioning

confidence: 99%

Highly Selective Silica‐supported Copper Catalysts Derived from Copper Phyllosilicates in the Hydrogenation of Adipic Acid to 1,6‐hexanediol

Jiang

Chen

et al. 2018

ChemCatChem

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Hydrogenation of adipic acid (AA) is a potential way to prepare 1,6‐hexanediol (HDOL). Herein, silica‐supported copper catalysts derived from copper phyllosilicates were synthesized, characterized, and tested in the hydrogenation of AA to HDOL. In a full conversion of AA, a high yield of HDOL (approximately 90 %) was obtained through the use of each Cu‐based catalyst. The turnover frequency calculated according to the consumption rate of AA was discovered to be dependent on the Cu+/(Cu0+Cu+) ratio and the reduction condition. Moreover, recycling tests showed that a catalyst derived from a copper phyllosilicate had better stability compared with Cu/SiO2 made through impregnation due to a stronger interaction between Cu and silica. The kinetic analyses based on the global rate expression and Langmuir−Hinshelwood−Hougen−Watson (LHHW) formalism of AA conversion were conducted. The possible competitive adsorption between AA and its derivatives, including hydroxycaproic acid and ϵ‐caprolactone, was thereby revealed.

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Section: Resultsmentioning

confidence: 99%

Highly Selective Silica‐supported Copper Catalysts Derived from Copper Phyllosilicates in the Hydrogenation of Adipic Acid to 1,6‐hexanediol

Jiang

Chen

et al. 2018

ChemCatChem

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“…Mostly, CuPS-cats are reduced at 300 or 350 °C to completely deconstruct Cu octahedral, to yield Cu + and Cu 0 species for catalysis applications. In some cases, lower reduction temperatures such as 200 [105], 220 [78], 250 [87,172], 260 [157], 270 [104,106], and 280 °C [84] were also selected for lower reduction degrees. The reduction temperatures and time are listed in Table 1.…”

Section: Reduction In Cups-catsmentioning

confidence: 99%

“…Taking FFAL [104,106] hydrogenation to FFOH for example, with proper catalyst design and operating condition, FFOH can be maximized as the desired product with limited extent of deep hydrogenation to 2-methylfuran (MF) [104,106] (Figure 25). In case of 5-hydroxymethylfurfural (HMF) [172] (Figure 25), the high conversion of HMF and 2,5-dihydroxymethylfuran (DHMF) yield can be obtained when UDP prepared CuPS-cats was applied. [104,106] and HMF to DHMF (adapted from [172]).…”

Section: Aldehyde To Alcoholmentioning

confidence: 99%

“…In case of 5-hydroxymethylfurfural (HMF) [172] (Figure 25), the high conversion of HMF and 2,5-dihydroxymethylfuran (DHMF) yield can be obtained when UDP prepared CuPS-cats was applied. [104,106] and HMF to DHMF (adapted from [172]).…”

Section: Aldehyde To Alcoholmentioning

confidence: 99%

“…Burgeoning research of CuPS-cats in the hydrogenation of other carbonyls such as carbonate [105,108,169,203,205], carboxylic acid [111,119,175], and aldehyde [104,106,160,172] have shown their potentials recently. Alternative applications of CuPScats, should be explored such steam reforming of DME [109,114,166], water-gas-shift reaction [206,207], dehydrogenation ethanol [98,202], dry reforming CH4 [136], ethynylation of formaldehyde [117].…”

Section: Challenges and Prospectivementioning

confidence: 99%

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Copper Phyllosilicates-Derived Catalysts in the Production of Alcohols from Hydrogenation of Carboxylates, Carboxylic Acids, Carbonates, Formyls, and CO2: A Review

Lin

2021

Catalysts

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Copper phyllosilicates-derived catalysts (CuPS-cats) have been intensively explored in the past two decades due to their promising activity in carbonyls hydrogenation. However, CuPS-cats have not been completely reviewed. This paper focuses on the aspects concerning CuPS-cats from synthesis methods, effects of preparation conditions, and dopant to catalytic applications of CuPS-cats. The applications of CuPS-cats include the hydrogenation of carboxylates, carboxylic acids, carbonates, formyls, and CO2 to their respective alcohols. Besides, important factors such as the Cu dispersion, Cu+ and Cu0 surface area, particles size, interaction between Cu and supports and dopants, morphologies, and spatial effect on catalytic performance of CuPS-cats are discussed. The deactivation and remedial actions to improve the stability of CuPS-cats are summarized. It ends up with the challenges and prospective by using this type of catalyst.

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Emerging Single‐Atom Catalysts/Nanozymes for Catalytic Biomedical Applications

Wang

2021

Adv Healthcare Materials

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Single-atom catalysts (SACs) are a type of atomically dispersed nanozymes with the highest atom utilization, which employ low-coordinated single atoms as the catalytically active sites. SACs not only inherit the merits of traditional nanozymes, but also hold high catalytic activity and superb catalytic selectivity, which ensure their tremendous application potential in environmental remediation, energy storage and conversion, chemical industry, nanomedicine, etc. Nevertheless, undesired aggregation effect of single atoms during preactivation and reaction processes is significantly enhanced owing to the high surface free energy of single atoms. In this case, appropriate substrates are requisite to prevent the aggregation event through the powerful interactions between the single atoms and the substrates, thereby stabilizing the high catalytic activity of the catalysts. In this review, the synthetic methods and characterization approaches of SACs are first described. Then the application cases of SACs in nanomedicine are summarized. Finally, the current challenges and future opportunities of the SACs in nanomedicine are outlined. It is hoped that this review may have implications for furthering the development of new SACs with improved biophysicochemical properties and broadened biomedical applications.

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Covalent-bonding to irreducible SiO2 leads to high-loading and atomically dispersed metal catalysts

Cited by 54 publications

References 59 publications

Highly Selective Silica‐supported Copper Catalysts Derived from Copper Phyllosilicates in the Hydrogenation of Adipic Acid to 1,6‐hexanediol

Highly Selective Silica‐supported Copper Catalysts Derived from Copper Phyllosilicates in the Hydrogenation of Adipic Acid to 1,6‐hexanediol

Copper Phyllosilicates-Derived Catalysts in the Production of Alcohols from Hydrogenation of Carboxylates, Carboxylic Acids, Carbonates, Formyls, and CO2: A Review

Emerging Single‐Atom Catalysts/Nanozymes for Catalytic Biomedical Applications

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