Small
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2023
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IF 13.3
Zhihao Chen,Malik Zeeshan Shahid,Xinyan Jiang,Meng Zhang,Danrui Pan,Hongpeng Xu,Guocan Jiang,Jin Wang,Zhengquan Li
Halide perovskites exhibit outstanding optoelectronic properties, which make them an ideal choice for photocatalytic CO 2 reduction and benzyl alcohol (BA) oxidation. Nevertheless, the simultaneous realization of the above redox coupling reactions on halide perovskites remains a great challenge, as it requires distinct catalytic sites for different target reactions. Herein, the catalytic sites of Cs 2 AgBiCl 6 (CABC) are regulated by doping Fe for efficient coupling of photocatalytic CO 2 reduction and BA oxidation. The Fe-doped CABC (Fe: CABC) exhibits an enhanced visible-light response and effective charge separation. Experimental results and theoretical calculations reveal a synergistic interplay between Bi and Fe sites, where the Bi and Fe sites have lower activation energies toward CO 2 reduction and BA oxidation. Further investigations demonstrate that electrons and holes prefer to accumulate at the Bi site and Fe site under light irradiation, respectively, which creates favorable conditions for facilitating CO 2 reduction and BA oxidation. The resultant Fe: CABC achieves a high photocatalytic performance toward CO (18.5 µmol g −1 h −1 ) and BD (1.1 mmol g −1 h −1 ) generation, which surpasses most of the state-of-the-art halide photocatalysts. This work demonstrates a facile strategy for regulating the catalytic site for redox coupling reactions, which will pave a new way for designing halide perovskites for photocatalysis.
研究领域:
材料科学
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光催化化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2018
·
IF 6.759
Yujie Song,Hao Wang,Shijing Liang,Yan Yu,Liuyi Li,Ling Wu
The photoalkylation of nitroarenes with benzyl alcohols in one pot at room temperature and 1 atm N 2 was achieved over the Pd/H 1.07 Ti 1.73 O 4 ·H 2 O nanosheets. The sample shows efficient photocatalytic activity with high conversion of nitrobenzene (99%) and selectivity of secondary amine (85%). This flexible photocatalytic system is also applicable to other nitroarenes with high efficiency. Results of in situ FTIR, DRS, and in situ ESR revealed that the benzyl alcohol and nitrobenzene molecules can bind with the surface Lewis and Brønsted acid sites in the catalyst via the H O⋯Ti and NO 2 ⋯H O Ti species. The formation of surface coordination species results in not only the activation of reactant molecules via surface electron transfer, but also the expanded visible light absorption of the catalyst. Moreover, in situ ESR suggested that the surface coordination can also facilitate the formation of oxygen vacancies in catalysts, which can greatly promote the exposure of Lewis sites and enhance the activation of reactant molecules. Finally, a possible hydrogen transfer strategy over the sample is proposed on a molecular level.
研究领域:
化学
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材料科学
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DOI
高影响因子
Catalysts
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2023
·Vol. 13
·期 5
·864
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IF 3.9
Xiya Chen,Hangwei Jiang,Danlan Cui,Kun Lu,Xiao Kong,Junmeng Cai,Shirui Yu,Xingguang Zhang
In organic synthesis, it is important to control the selectivity target product with high purity and reduce the cost of energy and equipment for separation. This study investigated supported gold catalysts on biochar-modified titanate-based nanofibers in order to regulate the catalytic performances by biochar content and surface properties. The catalysts were characterized by SEM, TEM, XRD, XPS, ICP-OES, UV-Vis to confirm their morphology, particle size distribution of Au NPs, crystal structures, oxidation state of Au and other key elements, real Au loading, and optical properties. In the test of selective oxidation of benzyl alcohol to benzaldehyde, the biochar modification could improve the selectivity toward benzaldehyde. Moreover, the influence of catalyst calcination conditions, reaction time, reaction atmospheres, reaction temperatures and solvent were systematically investigated. These results are useful for peer researchers in rational catalyst design.Keywords:gold catalysts;selectivity regulation;selective oxidation;benzyl alcohol
研究领域:
催化化学
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材料科学
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DOI
高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 34
·e202301948
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IF 2.1
Hai-Bo Wu,Xian-Tai Zhou,Xiao-Wu Zhou,Yan-Xiong Fang
Graphical Benzoic acid has been proved to be an efficient catalyst for the ring-opening polymerization of ϵ-caprolactone under mild conditions. A monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. It is expected to realize the one-step preparing of poly (ϵ-caprolactone) through the direct aerobic oxidation of cyclohexanone. The development of a feasible industrial method for poly(ϵ-caprolactone) (PCL) preparation is great of significant and challenging. The bulk ring-opening polymerization of ϵ-caprolactone (ϵ-CL) using various organic acid catalysts and benzyl alcohol (BnOH) as the initiator was developed. Benzoic acid (BA) has been proved to be an efficient catalyst for the ROP of ϵ-CL under mild conditions. The conversion of ϵ-CL to PCL was 84.7 % under the optimized reaction conditions, with number-average molecular weight ( M n ) and dispersity (PDI) of 7700 g/mol and 1.25, respectively. Moreover, a monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. Overall, this work is expected to provide a feasible industrial method for the preparation of PCL using benzoic acid as organocatalyst.
研究领域:
高分子化学
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有机催化
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产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2015
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IF 2.037
Hui Wang,Qinbo Wang,Zhenhua Xiong,Chuxiong Chen,Binwei Shen
By using the synthetic method, the solubilities of benzoic acid in binary methylbenzene + benzyl alcohol solvent mixtures at (301.05 to 355.65) K and in binary methylbenzene + benzaldehyde solvent mixtures at (301.05 to 354.45) K were determined at atmospheric pressure. The studied mass fractions of benzyl alcohol and benzaldehyde in the corresponding binary solvent mixtures range from 0.0 to 1.0. It was found that the measured solubilities increase with the increase of temperature at constant solvent composition. For the ternary system benzoic acid + methylbenzene + benzyl alcohol, the results show that the binary methylbenzene + benzyl alcohol solvent mixture with the mass fraction of benzyl alcohol at 0.80 has the best dissolving capacity for benzoic acid at constant temperature. However, for the ternary system benzoic acid + methylbenzene + benzaldehyde, the results show that the binary methylbenzene + benzaldehyde solvent mixture with the mass fraction of benzaldehyde of 0.20 has the best dissolving capacity for benzoic acid at constant temperature. The experimental data were correlated by both the nonrandom two-liquid (NRTL) and the Apelblat equations, and the correlated solubilities agree satisfactorily with the experimental observations. By coupling the Apelblat equation with the Clark and Glew equation, the thermodynamic functions for the two studied solid–liquid equilibrium systems, including dissolution enthalpy, entropy, Gibbs energy, and isobaric heat capacity, were calculated and discussed.
研究领域:
物理化学
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热力学
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DOI
高影响因子
Polymers
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2018
·Vol. 10
·期 10
·1089
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IF 2.935
Lili Liu,Xiaojing Zhou,Yongmei Yan,Jie Zhou,Wenping Zhang,Xishi Tai
The metal-organic zeolite imidazolate framework-8 (ZIF-8) supported gold-silver bimetallic catalysts with a core-shell structure (Au@Ag/ZIF-8 and Ag@Au/ZIF-8) and cluster structure (AuAg/ZIF-8) were successfully prepared by the deposition-redispersion method. Energy dispersive X-ray spectroscopy (EDS) elemental mapping images displayed that in the Au@Ag/ZIF-8 catalyst, Ag atoms were deposited on an exposed Au surface, and core-shell structured Au@Ag particles with highly dispersed Ag as the shell were formed. Additionally, the XPS investigation at gold 4f levels and silver 3d levels indicated that the Au and Ag particles of Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were in a zero valence state. Among the resultant catalysts obtained in this study, Ag@Au/ZIF-8 catalysts showed the highest catalytic activity for the selective oxidation of benzyl alcohol, followed by AuAg/ZIF-8 and Au@Ag/ZIF-8. The turnover frequency (TOF) values were in the order of Ag@Au/ZIF-8 (28.2 h−1) > AuAg/ZIF-8 (25.0 h−1) > Au@Ag/ZIF-8 (20.0 h−1) at 130 °C within 1 h under 8 bar O2when using THF as solvent. The catalysts of Au@Ag/ZIF-8 and Ag@Au/ZIF-8 with core–shell structures have higher benzaldehyde selectivities (53.0% and 53.3%) than the AuAg/ZIF-8 catalyst (35.2%) in the selective oxidation of benzyl alcohol into benzaldehyde. The effect of the solvent, reaction temperature, reaction time, and reaction pressure on benzyl alcohol conversion and benzaldehyde selectivity in benzyl alcohol selective oxidation over Au@Ag/ZIF-8, Ag@Au/ZIF-8, and AuAg/ZIF-8 were also investigated. All of the catalysts showed excellent performance at 130 °C under 8 bar O2within 1 h when using THF as the solvent in the selective oxidation of benzyl alcohol to benzaldehyde. Moreover, the catalysts can be easily recycled and used repetitively at least four times.Keywords:metal-organic frameworks;core-shell;bimetallic catalyst;aerobic oxidation;benzyl alcohol
研究领域:
催化化学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2018
·
IF 6.759
Weiwei Yu,Xinwen Guo,Chunshan Song,Zhongkui Zhao
The controlled visible-light mediated conversion of nitroaromatics to versatile nitrogen-containing intermediates is of great significance but still remains a challenge. Herein, we report for the first time a facile visible-light-initiated one-pot strategy for clean and efficient synthesis of nitrone from nitrobenzene and benzyl alcohol. It integrates the controlled photocatalytic reduction of nitrobenzene to phenylhydroxylamine by photogenerated electrons with the selective photocatalytic oxidation of benzyl alcohol to benzaldehyde by photoinduced holes over a low-cost CdS photocatalyst with a suitable reduction capability, followed by spontaneous condensation of the as-formed hydroxylamine and aldehyde at ambient pressure and room temperature. Furthermore, by modulating cocatalyst and illumination time, for the conversion of the same reactants, the other two useful nitrogen-containing compounds, imine and secondary amine, were also successfully synthesized. The reaction mechanisms for flexible synthesis of the three target products are proposed.
研究领域:
化学合成
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光催化反应
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产品关联
DOI
高影响因子
JOURNAL OF CHEMICAL RESEARCH
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2020
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IF 0.593
Zhenzhen Geng,Hong-yu Zhang,Guohui Yin,Yuecheng Zhang,Jiquan Zhao
The ionic liquid 1-methyl-3-(3-sulfopropyl)imidazolium chloride ([MIMPs]+Cl-) in combination with 2,2,6,6-tetramethylpiperidine-1-oxyl (TEMPO) and sodium nitrite (NaNO2) as a catalytic system demonstrates high efficiency in the one-pot two-step aerobic oxidative condensation of benzyl alcohols with 1,2-phenylenediamines to give benzimidazoles. Various benzimidazoles are obtained in good to excellent yields by this strategy.
研究领域:
有机化学
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催化化学
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DOI
高影响因子
ChemCatChem
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2020
·Vol. 12
·期 8
·2341-2347
·
IF 4.853
Bai-Chuan Zhou,Qing-Nan Wang,Xue-Fei Weng,Lei He,Wen-Cui Li,An-Hui Lu
Graphical Direct production of benzyl alcohol : The distribution of aromatic alcohols on cobalt-hydroxyapatite is greatly switched from methylbenzyl alcohol (feeding ethanol) to benzaldehyde (C 7 , BA=O) and benzyl alcohol (C 7 , BA−OH) by cofeeding of methanol and ethanol. Aromatic alcohols, often used for the synthesis of plasticizers, coatings and pharmaceuticals, are currently produced from the oxidation of petroleum-derived aromatic hydrocarbons. Herein, we report a non-petroleum and environmentally friendly route for the production of aromatic alcohols: cofeeding methanol with ethanol over cobalt-hydroxyapatite catalyst, in which the distribution of aromatic alcohols products can be regulated by varying methanol pressure. Co species on hydroxyapatite can activate both methanol and ethanol to yield their corresponding aldehydes (formaldehyde and acetaldehyde). The followed cross- and self-condensations of aldehydes are catalyzed by hydroxyapatite to produce acrolein and 2-butenal, which are the key intermediates for the formation of aromatic oxygenates. The sequential cross-condensation and dehydrocyclization of acrolein and 2-butenal yield benzaldehyde, which is then hydrogenated to benzyl alcohol. The direct production of benzyl alcohol from methanol and ethanol could be regarded as a cutting-edge example, which ensures a promising route for sustainable aromatic alcohols production.
研究领域:
化学工程
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催化科学
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环境科学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Xianglin Xiang,Bicheng Zhu,Jianjun Zhang,Chenhui Jiang,Tao Chen,Huogen Yu,Jiaguo Yu,Linxi Wang
The sluggish oxygen evolution reaction (OER) is often the bottleneck of photocatalytic overall water splitting, greatly suppressing the hydrogen-production activity. Herein, the slow OER was replaced by selective benzyl alcohol (BA) oxidation to benzaldehyde (BD) to promote H 2 production. The photocatalytic reaction was conducted over CdS quantum dots , which were modified with Co 2+ hole cocatalysts to further accelerate the rate-limiting BA oxidation. The photocatalytic system exhibits an ultra-high H 2 -production rate of 257.8 mmol g −1 h −1 with a remarkable apparent quantum yield of 69.3% under 365-nm light irradiation. The high performance is attributed to the Co 2+ hole cocatalysts on CdS surfaces, which not only enhance light absorption but also facilitate photogenerated carrier transfer. More importantly, both photogenerated electrons and holes are fully utilized in meaningful reactions. This work exemplifies a bifunctional photocatalytic system for simultaneous production of self-separated hydrogen and benzaldehyde, both of which are important industrial products.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 7
·1554
·
IF 4.2
Haorui Gong,Sai An,Weilong Qin,Yongbo Kuang,Deyu Liu
In order to expand the application of bismuth vanadate (BiVO4) to the field of photoelectrochemistry, researchers have explored the potential of BiVO4in catalyzing or degrading organic substances, potentially presenting a green and eco-friendly solution. A study was conducted to investigate the impact of electrolytes on the photocatalysis of benzyl alcohol by BiVO4. The research discovered that, in an acetonitrile electrolyte (pH 9) with sodium bicarbonate, BiVO4catalyzed benzyl alcohol by introducing saturated V5+. This innovation addressed the issue of benzyl alcohol being susceptible to catalysis in an alkaline setting, as V5+was prone to dissolution in pH 9 on BiVO4. The concern of the photocorrosion of BiVO4was mitigated through two approaches. Firstly, the incorporation of a non-aqueous medium inhibited the formation of active material intermediates, reducing the susceptibility of the electrode surface to photocorrosion. Secondly, the presence of saturated V5+further deterred the leaching of V5+. Concurrently, the production of carbonate radicals by bicarbonate played a vital role in catalyzing benzyl alcohol. The results show that, in this system, BiVO4has the potential to oxidize benzyl alcohol by photocatalysis.
研究领域:
光电化学
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催化
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Mingchuang Shen,Yingzhang Shi,Zhiwen Wang,Taikang Wu,Ling Hu,Ling Wu
Ultrathin Bi 4 Ti 3 O 12 nanosheets (NS) with the thickness about 3.9 nm were successfully synthesized by a hydrothermal method and were used as a photocatalyst for the oxidation of benzyl alcohol (BA) to benzaldehyde (BAD). The photocatalytic performance of NS is about 8 times higher than that of bulk Bi 4 Ti 3 O 12 . In-situ FTIR of pyridine adsorption and NH 3 -TPD reveal that NS has more surface Lewis acid sites (Ti 4+ ) for the adsorption and activation of BA. The photogenerated electrons (e - ) and holes (h + ) of NS can be fully used to produce the superoxide radicals and carbon-centered radicals, respectively. The monolayer nanosheet structure of NS not only greatly promotes the separation of photogenerated carriers, but also achieves the efficient activation of BA molecules via the C O⋯Ti coordination. This work successfully reveals the surface/interface interactions between the surface active sites of a photocatalyst and the reactive molecules via using ultrathin nanosheet as a molecular platform.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
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