Promoting inherent catalytic activity and stability of TiO2 supported Pt single-atoms at CeOx-TiO2 interfaces

Author(s):  
Mi Yoo ◽  
Eunji Kang ◽  
Hyuk Choi ◽  
Hyunwoo Ha ◽  
Han Seul Choi ◽  
...  

Single-atoms Single-atoms (SAs) with atomically coordinated reaction centers are considered the next generation catalyst that can reveal exceptional catalytic efficiency. However, the general concern about thermodynamic vulnerabilities of the SAs...

Catalysts ◽  
2021 ◽  
Vol 11 (1) ◽  
pp. 135
Author(s):  
Zhibin Wen ◽  
Qianqian Zhu ◽  
Jiali Zhou ◽  
Shudi Zhao ◽  
Jinnan Wang ◽  
...  

Novel flower-shaped C-dots/Co3O4{111} with dual-reaction centers were constructed to improve the Fenton-like reaction activity and peroxymonosulfate (PMS) conversion to sulfate radicals. Due to the exposure of a high surface area and Co3O4{111} facets, flower-shaped C-dots/Co3O4{111} could provide more Co(II) for PMS activation than traditional spherical Co3O4{110}. Meanwhile, PMS was preferred for adsorption on Co3O4{111} facets because of a high adsorption energy and thereby facilitated the electron transfer from Co(II) to PMS. More importantly, the Co–O–C linkage between C-dots and Co3O4{111} induced the formation of the dual-reaction center, which promoted the production of reactive organic radicals (R•). PMS could be directly reduced to SO4−• by R• over C-dots. On the other hand, electron transferred from R• to Co via Co–O–C linkage could accelerate the redox of Co(II)/(III), avoiding the invalid decomposition of PMS. Thus, C-dots doped on Co3O4{111} improved the PMS conversion rate to SO4−• over the single active site, resulting in high turnover numbers (TONs). In addition, TPR analysis indicated that the optimal content of C-dots doped on Co3O4{111} is 2.5%. More than 99% of antibiotics and dyes were degraded over C-dots/Co3O4{111} within 10 min. Even after six cycles, C-dots/Co3O4{111} still remained a high catalytic activity.


2010 ◽  
Vol 24 (31) ◽  
pp. 6115-6127 ◽  
Author(s):  
MARYAMOSSADAT BOZORGTABAR ◽  
MEHDI SALEHI ◽  
MOHAMMADREZA RAHIMIPOUR ◽  
MOHAMMADREZA JAFARPOUR

Titanium dioxide coatings were deposited by utilizing atmospheric plasma-spraying system. The agglomerated P25/20 nano-powder and different spraying parameters (e.g., Argon flow rate and spray distance) were used to determine their influences on the microstructure, crystalline structure, photo-absorption, and photo-catalytic performance of the coatings. The microstructure and phases of as-sprayed TiO 2 coatings were characterized by scanning electron microscope SEM and X-ray diffraction, respectively. Surface characteristics were investigated by Fourier Transform Infrared. Photo-catalytic efficiency of the elaborated samples was also determined in an environmental test chamber set-up and evaluated from the conversion rate of ethanol. The photo-absorption was determined by UV–Vis spectrophotometer. The as-sprayed TiO2 coating was photo-catalytically reactive for the degradation of ethanol. The photo-catalytic activity was influenced by spray conditions. It is found that the photo-catalytic activity is significantly influenced by anatase content, surface area, and surface state. The results showed that the argon flow rate has an influence on the microstructure, anatase content, and photo-catalytic activity of the TiO 2 coatings.


2019 ◽  
Vol 6 (2) ◽  
pp. 171-176
Author(s):  
Rajasekhar Dodda ◽  
Sampak Samanta ◽  
Matthew Su ◽  
John Cong-Gui Zhao

Background: While proline can catalyze the asymmetric direct aldol reactions, its catalytic activity and catalyst turnover are both low. To improve the catalytic efficiency, many prolinebased organocatalysts have been developed. In this regard, prolinamide-based bifunctional catalysts have been demonstrated by us and others to be highly efficient catalysts for the direct aldol reactions. Results: Using the β-acetamido- and β-tosylamidoprolinamide catalysts, the highly enantio- and diastereoselective direct aldol reactions between enolizable ketones and aldehydes were achieved (up to >99% ee, 98:2 dr). A low catalyst loading of only 2-5 mol % of the β-tosylamidoprolinamide catalyst was needed to obtain the desired aldol products in good to high yields and high stereoselectivities. Methods: By carefully adjusting the hydrogen bonding ability of the remote β-amide hydrogen of the 1,2-diamine-based prolinamide bifunctional catalysts, the catalytic activity and the asymmetric induction of these catalysts were significantly improved for the direct aldol reaction between aldehydes and enolizable ketones. Conclusion: Some highly efficient 1,2-diamine-based bifunctional prolinamide catalysts have been developed through probing the remote β-amide hydrogen for its hydrogen bonding capability. These catalysts are easy to synthesize and high enantioselectivities may be achieved at very low catalyst loadings.


2019 ◽  
Vol 5 (8) ◽  
pp. eaaw2322 ◽  
Author(s):  
Peng Peng ◽  
Lei Shi ◽  
Feng Huo ◽  
Chunxia Mi ◽  
Xiaohong Wu ◽  
...  

Nitrogen-coordinated single-atom catalysts (SACs) have emerged as a frontier for electrocatalysis (such as oxygen reduction) with maximized atom utilization and highly catalytic activity. The precise design and operable synthesis of SACs are vital for practical applications but remain challenging because the commonly used high-temperature treatments always result in unpredictable structural changes and randomly created single atoms. Here, we develop a pyrolysis-free synthetic approach to prepare SACs with a high electrocatalytic activity using a fully π-conjugated iron phthalocyanine (FePc)–rich covalent organic framework (COF). Instead of randomly creating Fe-nitrogen moieties on a carbon matrix (Fe-N-C) through pyrolysis, we rivet the atomically well-designed Fe-N-C centers via intermolecular interactions between the COF network and the graphene matrix. The as-synthesized catalysts demonstrate exceptional kinetic current density in oxygen reduction catalysis (four times higher than the benchmark Pt/C) and superior power density and cycling stability in Zn-air batteries compared with Pt/C as air electrodes.


2018 ◽  
Vol 42 (24) ◽  
pp. 19740-19748 ◽  
Author(s):  
Longgang Wang ◽  
Jin Zhang ◽  
Xiaolei Guo ◽  
Shengfu Chen ◽  
Yanshuai Cui ◽  
...  

This study offers a method for constructing an artificial enzyme (Pdn-G5MC), which maintains its catalytic efficiency in bacterial solution.


Nanomaterials ◽  
2018 ◽  
Vol 8 (12) ◽  
pp. 963
Author(s):  
Wei Liu ◽  
Xiaolian Zhu ◽  
Chengcheng Xu ◽  
Zhao Dai ◽  
Zhaohui Meng

A new AuNPs-based thermosensitive nanoreactor (SiO2@PMBA@Au@PNIPAM) was designed and prepared by stabilizing AuNPs in the layer of poly(N,N’-methylenebisacrylamide) (PMBA) and subsequent wrapping with the temperature-sensitive poly(N-isopropylacrylamide) (PNIPAM) layer. The new nanoreactor exhibited high dispersibility and stability in aqueous solution and effectively prevented the aggregation of AuNPs caused by the phase transformation of PNIPAM. The XPS and ATR-FTIR results indicated that AuNPs could be well stabilized by PMBA due to the electron transfer between the N atoms of amide groups in the PMBA and Au atoms of AuNPs. The catalytic activity and thermoresponsive property of the new nanoreactor were invested by the reduction of the environmental pollutant, 4-nitrophenol (4-NP), with NaBH4 as a reductant. It exhibited a higher catalytic activity at 20 °C and 30 °C (below LCST of PNIPAM), but an inhibited catalytic activity at 40 °C (above LCST of PNIPAM). The PNIPAM layer played a switching role in controlling the catalytic rate by altering the reaction temperature. In addition, this nanoreactor showed an easily recyclable property due to the existence of a silica core and also preserved a rather high catalytic efficiency after 16 times of recycling.


Catalysts ◽  
2019 ◽  
Vol 9 (12) ◽  
pp. 1053 ◽  
Author(s):  
Manas Sutradhar ◽  
Tannistha Roy Barman ◽  
Armando J. L. Pombeiro ◽  
Luísa M. D. R. S. Martins

The mononuclear Cu(II) complex [Cu((kNN′O-HL)(H2O)2] (1) was synthesized using N-acetylpyrazine-2-carbohydrazide (H2L) and characterized by elemental analysis, IR spectroscopy, ESI-MS and single crystal X-ray crystallography. Two Fe(III) complexes derived from the same ligand viz, mononuclear [Fe((kNN′O-HL)Cl2] (2) and the binuclear [Fe(kNN′O-HL)Cl(μ-OMe)]2 (3) (synthesized as reported earlier), were also used in this study. The catalytic activity of these three complexes (1–3) was examined towards the oxidation of alcohols using tert-butyl hydroperoxide (TBHP) as oxidising agent under solvent-free microwave irradiation conditions. Primary and secondary benzyl alcohols (benzyl alcohol and 1-phenylethanol), and secondary aliphatic alcohols (cyclohexanol) were used as model substrates for this study. A comparison of their catalytic efficiency was performed. Complex 1 exhibited the highest activity in the presence of TEMPO as promoter for the oxidation of 1-phenylethanol with a maximum yield of 91.3% of acetophenone.


2020 ◽  
Vol 59 (46) ◽  
pp. 20691-20696 ◽  
Author(s):  
Hojin Jeong ◽  
Dongjae Shin ◽  
Beom‐Sik Kim ◽  
Junemin Bae ◽  
Sangyong Shin ◽  
...  

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