SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Ting Zhang,Weitao Wang,Meng He,Huan Wang,Zhen-Hong He,Yang Yang,Kuan Wang,Zhao-Tie Liu
Imines as valuable chemical intermediates can be synthesized by aerobic photocatalytic oxidation of amines, which is recognized as a promising and green route for imines synthesis. It is attractive to develop solvent-free photocatalytic oxidation of amines with high efficiency, especially with high activity and selectivity, but it is challenging. In the present work, flower-like BiOX/TiO 2 (X = Cl, Br, I) heterojunction was designed for solvent-free photocatalytic oxidation of benzylamine to N-benzylidenebenzylamine. Type II heterojunction of BiOCl/TiO 2 with 67.3 wt% of BiOCl achieved the high formation rate of 6316 µmol∙g −1 ∙h −1 and selectivity of 99 % on BiOCl/TiO 2 . To the best of our knowledge, the activity and selectivity are the highest for solvent-free photocatalytic system. The reason for the varied photocatalytic performances were investigated. The solvent-free photocatalytic mechanism was revealed and proposed. Moreover, the BiOCl/TiO 2 photocatalyst can be used for photocatalytic oxidation of varied benzylamines to imines.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Micromachines
·
2022
·Vol. 13
·期 11
·1857
·
IF 3.523
Shisong Yu,Kai Zhang,Xiangcheng Cai,Peng Tu,Yuanming Zhou,Fei Mei
Organic-inorganic perovskite materials are widely used in the preparation of light-emitting diodes due to their low raw material cost, solution preparation, high color purity, high fluorescence quantum yield, continuously tunable spectrum, and excellent charge transport properties. It has become a research hotspot in the field of optoelectronics today. At present, the nonradiative recombination and fluorescence quenching occurring at the interface between the device transport layer and the light-emitting layer are still important factors limiting the performance of perovskite light-emitting diodes (PeLEDs). In this work, based on CH3NH3PbBr3perovskite, the effects of parameters such as precursor solution, anti-solvent chlorobenzene (CB), and small amine molecule phenylmethylamine (PMA) on the performance of perovskite films and devices were investigated. The research results show that adding an appropriate amount of PMA can reduce the grain size of perovskite, improve the coverage of the film, enhance the crystallinity of the film, and increase the fluorescence intensity of the perovskite film. When the PMA content is 0.050 vol.%, the maximum luminance of PeLEDs is 2098 cd/m2and the maximum current efficiency is 1.592 cd/A, which is greatly improved by 30% and 64.8% compared with the reference device without PMA doping. These results suggest that an appropriate amount of PMA can effectively passivate the defects in perovskite films, and inhibit the non-radiative recombination caused by the traps, thereby improving the optoelectronic performance of the device.Keywords:perovskite;phenylmethylamine;chlorobenzene;light-emitting diode
研究领域:
材料科学
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光学工程
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产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
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2022
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IF 5.436
Zhi Hua Zhang,Li Xia Chen,Yun Qian Zhang,Qian Jiang Zhu,Kai Chen,Zhu Tao
The anion-induced outer surface interaction of Q[n]s is an important driving force in the construction of Q[n]-based supramolecular frameworks. In this work, a symmetric tetramethyl-substituted cucurbit[6]uril (TMeQ[6]) is selected as the basic structural block. Using the anion-induced outer surface interaction of Q[n]s derived from [CdxCly]n− anions formed by Cd2+ cations in a HCl medium, four different TMeQ[6]-[CdxCly]n−-based supramolecular frameworks are constructed. Three of the most common TMeQ[6]-[CdxCly]n−-based supramolecular frameworks are selected for further vulcanization, and three different CdS/TMeQ[6]-based framework catalysts with different structures and properties are obtained. The catalytic activities of these three CdS/TMeQ[6]-based framework catalysts are investigated by the coupling photocatalytic reaction of aminobenzyl, and the results showed that the catalytic activities of the three catalysts are all higher than that of pure CdS. Therefore, this work establishes that it is possible to establish a method for synthesizing the Q[n]-based framework-supported catalysts by first synthesizing TMeQ[6]-[CdxCly]n−-based supramolecular frameworks and then forming Q[n]-based framework supported catalysts by sulfurization or reduction.
研究领域:
材料科学
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催化化学
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DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2025
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IF 4.7
Jing Xu,Kangle Wan,Jianjie Wu,Yunchao Wu,Wei Yan,Lichuan Zhang,Yuanping Chen,Yingcong Wei
During the piezoelectric photocatalytic process, the surface curvature of the piezoelectric photocatalyst undergoes dynamic changes under the influence of external mechanical forces. However, the correlation between the surface curvature and catalytic performance remains largely unexplored. Here, we demonstrate that decreasing the radius of curvature of MoSe2 significantly enhances its piezoelectric-photocatalytic activity for C–N coupling reactions, enabling imine synthesis from benzylamine. Comprehensive characterization and DFT calculations together show that the piezoelectric effect in the curved MoSe2 structure inhibits photogenerated charge carriers from recombination, improving carrier utilization efficiency. Additionally, the surface curvature effect induced by ultrasonic driving reduces the band gap. It promotes the effective transfer of electrons from Mo atoms in MoSe2 to −NH2 in benzylamine, thereby facilitating the activation of the benzylamine molecule. As a result, the synergistic effects of the piezoelectric and curvature characteristics significantly enhance the photocatalytic performance of MoSe2 toward the C–N coupling of benzylamine. This study not only provides new insights into interfacial reaction mechanisms in piezoelectric photocatalysis but also offers a novel perspective for designing high-performance catalytic systems.
研究领域:
材料科学
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催化化学
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理论计算
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DOI
PubMed
高影响因子
CHINESE JOURNAL OF CHEMISTRY
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2020
·Vol. 38
·期 11
·1292-1298
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IF 3.826
Chuanchuan Zhao,Yongjun Gao,Ziyi Zhang,Ding Ma
Summary of main observation and conclusion Sustainable phytic acid and cellulose are selected as precursors to fabricate P-doped carbon material (C-P-500), which possesses the high surface area and exhibits excellent catalytic activity and stability in the oxidative coupling of benzylamines (conversion > 95%, yield > 95%). During the carbonization of cellulose in the muffle furnace, phytic acid can efficiently prevent the cellulose-derived carbon from combustion and create micro/meso porous structure because of its special function of fire retardation. Control experiments and characterizations demonstrate that P-containing groups anchoring on C-P-500 improve the catalytic performance of carbocatalyst in the oxidation of benzylamines to imines. The excellent catalytic activity of C-P-500 should be contributed collectively by carbonyl and P=O(OH) 2 groups. Due to the sustainable property of precursors and simple methodology for fabricating P-doped carbocatalyst, along with the moderate reaction conditions, it is a green catalytic system for the oxidative coupling of benzylamines to imines.
研究领域:
化学
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可持续化学
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催化科学
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DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Jinbiao Shi,Jianling Zhang,Tongling Liang,Dongxing Tan,Xiuniang Tan,Qiang Wan,Xiuyan Cheng,Bingxing Zhang,Buxing Han,Lifei Liu,Fanyu Zhang,Gang Chen
Metal–organic frameworks (MOFs) have attracted increased research attention in photocatalysis due to their great potential in light harvest and conversion. However, the organic transformations as photocatalyzed by MOFs under mild conditions yet remain a challenge. Herein, three bipyridyl-containing cadmium–organic frameworks Cd(dcbpy) (dcbpy = 2,2′-bipyridine-5,5′-dicarboxylate), Cd(bdc)(bpy) (bdc = 1,4-benzenedicarboxylate; bpy = 2,2′-bipyridyl), and Cd(bdc)(2Me-bpy) (2Me-bpy = 4,4′-dimethyl-2,2′-bipyridyl) were synthesized for the first time. The bpy-containing Cd-MOFs have strong light harvest abilities and suitable photocatalysis energy potentials, making them highly active and selective for the photo-oxidation of benzylamine to N-benzylbenzaldimine under mild conditions, i.e., using atmospheric air as oxidant, at room temperature, and in the absence of any photosensitizer or cocatalyst. It provides an efficient, economical, and green way for the direct oxidation of amines to produce imines.
研究领域:
材料科学
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化学
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产品关联
DOI
PubMed
高影响因子
SEMICONDUCTOR SCIENCE AND TECHNOLOGY
·
2021
·Vol. 36
·期 7
·075004
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IF 2.352
Yefeng Chen,Dan Tang,Zhuhan Wang,Wen Li,Mengyun Yin,Qin Yang,Yafen Zhou,Kaiming Zhang,Taotao Kan,Limei Zhou
As an important intermediate, imine is widely used in industrial chemistry. The photocatalytic oxidation of amines to form imines is a green and economical method. But it remains a challenge for the efficient transformation under mild conditions. Herein, a Z-scheme carbon nitride (CM)-Fe2O3 heterojunction photocatalyst was synthesized by in-situ preparation of Fe2O3 nanoparticles on two-dimensional CM nanosheets. The as-prepared catalyst exhibited efficient photocatalysis activity in selective oxidation of benzylamine to N-benzylidene benzylamine. Under ambient air and room temperature, the selectivity and conversion rate both can reach 99.9%, and the corresponding turnover frequency value reaches up to 9.99 mmol g−1 h−1, superior to the most of heterogeneous photocatalysts reported in previous literatures. The excellent catalytic activity of the modified CM material may be due to the enhanced absorption of visible light and the improved photogenerated carrier separation and migration rate, and the Z-scheme mechanism also retains the strong oxidation and reduction ability of the composite material. This work will provide a promising and practical method to promote the photocatalytic conversion of solar-driven organics.
研究领域:
材料科学
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环境化学
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光催化技术
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DOI
高影响因子
RSC Advances
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2020
·Vol. 10
·期 47
·28059-28065
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IF 3.119
Yunqi Fu,Mang Zheng,Qi Li,Liping Zhang,Shuai Wang,V. V. Kondratiev,Baojiang Jiang
Benzylamine coupling is a very important reaction for the synthesis of imine but still faces many challenges. Herein, we present a highly effective strategy towards the coupling reaction by using environmentally friendly catalysts. These catalysts are composed of Cu/Cu2O/Cu3N heterostructures supported by C3N4 tubes and the composites were synthesized by one-step hydrothermal treatment followed by calcination. Cu2O, Cu3N, and C3N4 all are responsive to visible light and the heterojunction formed can greatly enhance the charge separation. When used as photocatalysts for oxidative self-coupling of benzylamine at a low temperature of 323 K in air, Cu/Cu2O/Cu3N/C3N4 was able to give conversion and selectivity values of up to 99% and 98%, respectively. The high efficiency of the catalysts is attributable to their ability to generate large quantities of free radicals (such as ·OH and ·O2−) under visible-light irradiation.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Journal of Materials Chemistry A
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2024
·Vol. 12
·期 18
·11020-11027
·
IF 10.7
Wenhao Zheng,Xiao Peng,Wenjing Zhai,Lin Huang,Peizhuo Chen,Penghui Shi,Xiaohui Zhou,Jianguo Wan,Zhibo Yan,J.-M. Liu
Tin-based halide perovskites have become the prospective photoelectric materials due to their remarkable optoelectronic properties and relatively low toxicity. However, the rapid crystallization and easy oxidation of Sn2+ to Sn4+ made it challenging to fabricate efficient photoelectric devices. Herein, benzylamine boron trifluoride (BBF) was introduced into the FASnI3 precursor solution to tune the crystal quality and photoelectric properties of FASnI3 films. It was demonstrated that the BBF passivates the film defects, reduces the content of Sn4+, enhances the PL intensity and stability, and improves the responsivity at wavelengths from 415 to 980 nm. The treatment of BBF with an optimal concentration of 1.5 mg mL−1 improves the responsivity of the device from 0.89 to 2.6 A W−1. The coordination of BBF with the anions/cations in the perovskite precursor is suggested to account for the improvement of crystal quality and the photoelectric properties of FASnI3 films.
研究领域:
材料科学
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光电子学
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DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Yu Ding,Bo-Qiang Miao,Shu-Ni Li,Yu-Cheng Jiang,Yan-Yan Liu,Hong-Chang Yao,Yu Chen
In this work, ultra-thin Ni 2 P nanomeshes (1.9 nm thickness) on nickel foam (NF) substrate (denoted as Ni 2 P-UNMs/NF) are successfully achieved through phosphidation treatment using ultra-thin Ni(OH) 2 nanomeshes on NF substrate (denoted as Ni(OH) 2 -UNMs/NF) as reaction precursor. Because of the sufficient active sites in edge of the holes, high specific surface area, porous framework and high conductivity of NF substrate, Ni 2 P-UNMs/NF nanocomposites show the outstanding activity for both hydrogen evolution reaction (HER) and benzylamine oxidation reaction (BOR) in alkaline electrolyte. Importantly, Ni 2 P-UNMs/NF nanocomposites can directly act as a bifunctional electrocatalyst for the electrochemical water-splitting in two electrode system in the presence of benzylamine, which only requires an electrolysis voltage of 1.41 V to achieve the 10 mA cm -2 current density in alkaline electrolyte, accompanying with H 2 production at cathode and value-added benzonitrile production at anode. Obviously, the BOR boosted electrochemical water-splitting provides an energy-saving and cost-competitive H 2 production method.
研究领域:
材料科学
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电化学
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能源转化
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产品关联
DOI
高影响因子
ACS Catalysis
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2025
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IF 13.1
Ren Ma,Yujing Zhang,Feiyang Yu,Shilong Wei,Yang Xing,Chengfang Qiao,Zhengqiang Xia,Qi Yang,Gang Xie,Sanping Chen
High energy level difference between electron donor (D) and electron acceptor (A) and low energy loss during charge transfer are prerequisites for the construction of efficient D–A-type covalent-organic framework (COF) photocatalysts. However, the spatial structure characteristics of the building blocks inevitably lead to the torsion of the D–A COF skeleton during the construction process and thus prevent effective charge migration. Herein, with the high-energy-level triphenylamine (TPA) as a model electron donor, the formyl positional isomers of tris(3-formylbiphenyl) amine (NDC) and tri(4-formylbiphenyl) amine (NBC) react with an acceptor 1,3,5-tris(4-aminophenyl) triazine (TTA), producing both D–A COFs for photocatalytic CO2 reduction and benzylamine coupling reactions. Structural investigations evidence that the formyl positional isomerism imparts the dihedral angle of TPA single arm reducing from 51.09 to 2.12°, the interlayer spacing from 3.89 to 3.55 Å, and the exciton binding energy from 97.25 to 85.86 meV in TTA-COFs. Such the “near-flat” TTA-NDC structure with confined clover-like channels dramatically accelerates the intralayer and interlayer charge migration efficiency and improves CO2 adsorption and oxygen activation ability (O2•– concentration of 48.01 μmol·L–1 in 3 h). To the best of our knowledge, TTA-NDC exhibits the highest benzylamine coupling efficiency with a turnover frequency value of 518.4 h–1 among the pristine COF photocatalysts, and its electron consumption rate for photocatalytic CO2 reduction reaches 1632.2 μmol·g–1·h–1, 3.85-fold higher than TTA-NBC, far surpassing most COF-based photocatalysts. Parallelly, the protonated H-TTA-NDC shows high CO2 reduction to CH4 yield (310.1 μmol·g–1·h–1) and selectivity (85.1%) due to the improved proton conductivity (σ = 1.07 × 10–2 S·cm–1). Additionally, the durability, stability, and possible photocatalytic mechanisms of TTA-NDC were systematically investigated.
研究领域:
材料科学
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光化学
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环境科学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2015
·Vol. 3
·期 35
·18045-18052
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IF 7.443
Yantao Zhang,Linjuan Pei,Zhanfeng Zheng,Yong Yuan,Tengfeng Xie,Juan Yang,Shuai Chen,Junwen Wang,Eric R. Waclawik,Huaiyong Zhu
The formation of heterojunctions between two crystals with different band gap structures, acting as a tunnel for the unidirectional transfer of photogenerated charges, is an efficient strategy to enhance the photocatalytic performance of semiconductor photocatalysts. Considering that surface complex photocatalysts also exhibit charge separation and recombination processes, the heterojunctions may also promote the visible-light-response photoactivity of any surface complex catalysts by influencing the transfer of photogenerated electrons. Herein, Nb2O5 microfibers, with a high surface area of interfaces between an amorphous phase and a crystalline phase, were designed and synthesised by the calcination of hydrogen-form niobate while controlling the crystallisation. The photoactivity of these microfibres towards selective aerobic oxidation reactions was investigated. As predicted, the Nb2O5 microfibres containing heterojunctions exhibited the highest photoactivity. This could be due to the band gap difference between the amorphous phase and the crystalline phase that allows electron transfer unidirectionally, which decreased the recombination rate and improved the efficiency.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）