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Journal of the Taiwan Institute of Chemical Engineers · 2019 · IF 3.834

Efficient synthesis of glucose into 5-hydroxymethylfurfural with SO42−/ZrO2 modified H+ zeolites in different solvent systems

Yunchao Feng,Miao Zuo,Ting Wang,Wenlong Jia,Xiaoyu Zhao,Xianhai Zeng,Yong Sun,Xing Tang,Tingzhou Lei,Lu Lin

Production of 5-hydroxymethylfurfural (HMF) from glucose with high yield remains a big challenge. Thereinto, assembling catalysts with outstanding performance is the bottleneck at the current stage. In this study, effective catalysts were synthesized by loading SO 4 2− /ZrO 2 (SZ) on a series of H + zeolites to investigate the catalytic dehydration of glucose into HMF. Among all the catalysts applied, 2-SZ-HM-550 (HZSM-5 with Si/Al molar ratios of 80∼150, calcined at 550 °C) gave the yields of HMF 41.32%, 61.14%, 54.67% and 40.71% in 4 applied reaction systems, respectively. Moreover, HMF with desirable yield was obtained while other carbohydrates were dehydrated catalyzed by 2-SZ-HM-550, such as fructose, sucrose, inulin and starch.

研究领域: 化学工程 · 催化科学
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Catalysts · 2018 ·Vol. 8 ·期 8 ·326 · IF 3.465

Modification to L-H Kinetics Model and Its Application in the Investigation on Photodegradation of Gaseous Benzene by Nitrogen-Doped TiO2

Peng Sun,Jun Zhang,Wenxiu Liu,Qi Wang,Wenbin Cao

In this paper, the Langmuir-Hinshelwood (L-H) model has been used to investigate the kinetics of photodegradation of gaseous benzene by nitrogen-doped TiO2(N-TiO2) at 25 °C under visible light irradiation. Experimental results show that the photoreaction coefficientkpmincreased from 3.992 × 10−6mol·kg−1·s−1to 11.55 × 10−6mol·kg−1·s−1along with increasing illumination intensity. However, the adsorption equilibrium constantKLdecreased from 1139 to 597 m3·mol−1when the illumination intensity increased from 36.7 × 104lx to 75.1 × 104lx, whereas it was 2761 m3·mol−1in the absence of light. This is contrary to the fact thatKLshould be a constant if the temperature was fixed. This phenomenon can be attributed to the breaking of the adsorption-desorption equilibrium by photocatalytically decomposition. To compensate for the disequilibrium of the adsorption-desorption process, photoreaction coefficientkpmwas introduced to the expression ofKLand the compensation form was denoted asKm.KLis an indicator of the adsorption capacity of TiO2whileKmis only an indicator of the coverage ratio of TiO2surface. The modified L-H model has been experimentally verified so it is expected to be used to predict the kinetics of the photocatalytic degradation of gaseous benzene.Keywords:modified L-H model;N-TiO2;photocatalytic degradation;benzene

研究领域: 环境科学 · 化学工程
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ACS Applied Materials & Interfaces · 2016 · IF 7.145

Influence of C–H···O Hydrogen Bonds on Macroscopic Properties of Supramolecular Assembly

Wei Ji,Guofeng Liu,Zijian Li,Chuanliang Feng

For CH···O hydrogen bonds in assembled structures and the applications, one of the critical issues is how molecular spatial structures affect their interaction modes as well as how to translate the different modes into the macroscopic properties of materials. Herein, coumarin-derived isomeric hydrogelators with different spatial structures are synthesized, where only nitrogen atoms locate at the ortho, meso, or para position in the pyridine ring. The gelators can self-assemble into single crystals and nanofibrous networks through CH···O interactions, which are greatly influenced by nitrogen spatial positions in the pyridine ring, leading to the different self-assembly mechanisms, packing modes, and properties of the nanofibrous networks. Typically, different cell proliferation rates are obtained on the different CH···O bonds driving nanofibrous structures, implying that tiny variation of the stereo-position of nitrogen atoms can be sensitively detected by cells. The study paves a novel way to investigate the influence of isomeric molecular assembly on macroscopic properties and functions of materials.

研究领域: 材料科学 · 生物学 · 医学
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CATALYSIS LETTERS · 2018 ·Vol. 148 ·期 11 ·3445-3453 · IF 2.911

Controllable Synthesis of MoS2/h-CdS/c-CdS Nanocomposites with Enhanced Photocatalytic Hydrogen Evolution Under Visible Light Irradiation

Li Xia,Dong Hao,Wang Bo,Lv Jun,Xu Guangqing,Wang Dongmei,Wu Yucheng

Firstly, h-CdS/c-CdS homojunction was prepared by solvothermal method with controlling the Cd-to-S molar ratio. Then, the MoS 2 /h-CdS/c-CdS nanocomposites were constructed by ultrasonic method with different MoS 2 amount. The experimental results showed that when the molar ratio of Cd and S was 1:1 and the amount of MoS 2 was 1.5 wt%, the MoS 2 /h-CdS/c-CdS nanocomposites exhibited excellent photocatalytic performance for hydrogen evolution under visible light. The total amount of hydrogen evolution was 3753.12 µmol for 5 h, and its average hydrogen evolution rate was 40.79 mmol h −1  g −1 with an apparent quantum efficiency of 38.16% irradiated at 420 nm, which was about 7.3 times when compared with the h-CdS/c-CdS homojunction (Cd:S = 1:8). The enhanced photocatalytic performance of MoS 2 /h-CdS/c-CdS could be attributed to the improved specific surface area and formation of well bonded interface structure, which not only enhanced the response to visible light but also decreased the recombination rates of photogenerated charge carriers. Graphical Abstract

研究领域: 材料科学 · 光催化
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CEMENT AND CONCRETE RESEARCH · 2024 · IF 10.9

Ca/Si-dependent size of silica nanoparticles derived from C-S-H at high water to solid ratio

Binmeng Chen,Xu Fang,Yuyang Zhao,Zongjin Li

In recycling and reusing construction waste, carbonation of recycled concrete fine (RCF) has been successfully applied to produce value-added products, such as silica nanoparticles, via the breaking of calcium silicate hydrate (C-S-H) structure and condensation of silicate chains. However, the intricacies of carbonation of RCF with varying calcium to silicon (C/S) ratios and their implications on the size of generated silica nanoparticles remain unknown. In this work, we developed an optimized carbonation method at high water to solid ratio to fabricate silica nanoparticles from C-S-H with different C/S ratios. The particle size of silica nanoparticles was found to gradually decrease with the increased C/S ratio of C-S-H. Since as C/S ratio increased, silicate in Q 3 state shifted to Q 1 state and the silicate chain became shorter, shifting from long-range, disordered to short-range, ordered. As the disordered self-seeding growth of long silicate chains derived from C-S-H continued, the Si-O-Si network of silica nanoparticles became chaotic, leaving more unreacted Si-OH on its surface. On the contrary, the short silicate chains displayed higher possibility of condensation, making nanoparticles with a smaller diameter.

CAS / MDL: 1305-62-0
研究领域: 材料科学 · 环境工程
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CHINESE JOURNAL OF CHEMICAL ENGINEERING · 2021 · IF 3.171

Efficient conversion of benzene and syngas to toluene and xylene over ZnO-ZrO2&H-ZSM-5 bifunctional catalysts

Xiao Zhao,Xuan Shi,Zhongshun Chen,Long Xu,Chengyi Dai,Yazhou Zhang,Xinwen Guo,Dongyuan Yang,Xiaoxun Ma

A series of ZnO-ZrO 2 solid solutions with different Zn contents were synthesized by the urea co-precipitation method, which were coupled with H-ZSM-5 zeolite to form bifunctional catalysts. As a new benzene alkylation reagent, syngas was used instead of methanol to realize the efficient conversion of syngas and benzene into toluene and xylene. A suitable ratio of ZnO-ZrO 2 led to the significant improvement in the catalytic performance, and a suitable amount of acid helped to increase the selectivity of toluene/xylene and reduce the selectivity of the by-products ethylbenzene and C 9 + aromatics. The highest benzene conversion of 89.2% and toluene/xylene selectivity of 88.7% were achieved over 10% ZnO-ZrO 2 &H-ZSM-5 (Si/Al = 23) at a pressure of 3 MPa and a temperature of 450 °C. In addition, the effect of the zeolite framework structure on product distribution was examined. Similar to the molecular dynamics of aromatic hydrocarbons , H-ZSM-5 zeolites comprise 10-membered-ring pores, which are beneficial to the activation of benzene; hence, the conversion of benzene is higher. H-ZSM-35 and H-MOR zeolites exhibited small eight-membered-ring channels, which were not conducive to the passage of benzene; hence, the by-product ethylbenzene exhibits a higher selectivity. The distance between the active centers of the bifunctional catalysts was the main factor affecting the catalytic performance, and the powder mixing method was more conducive to the conversion of syngas and benzene.

CAS / MDL: 10196-18-6
研究领域: 催化化学 · 材料科学
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JOURNAL OF CATALYSIS · 2023 · IF 7.3

Defective Auδ−-Ov interfacial sites boost C-H bond activation for enhanced selective oxidation of amino alcohols to amino acids

Ying Liao,Yue Pan,Xiang Feng,Xiaobo Chen,Yibin Liu,Chaohe Yang,Hao Yan

Designing efficient active sites to facilitate the oxidation of hydroxyl group to carboxylic acid under the influence of nitrogen-containing functional groups is worth exploring, but it is rarely investigated. Herein, we construct defective Au-ZrO 2 interfacial structures by tuning the calcination temperature of ZrO 2 support to boost the oxidation of amino alcohols to amino acids. Interestingly, the modification of calcination temperature induces the escape of saturated coordination oxygen atoms in ZrO 2 support, leaving behind abundant surface oxygen vacancy (O v ). The as-formed Au δ− -O v interfacial site displays the unique synergistic adsorption effect and electron transfer ability. Specifically, the O v site voluntarily adsorbs the –NH 2 group of amino alcohol, thus ensuring that the electron-rich Au δ− nearby O v site adsorbs the hydroxyl groups and activates the C-H bond activation of NH 2 CH 2 CH 2 O* intermediates. Consequently, Au/ZrO 2 -600 catalyst with more defective Au δ− -O v interfacial sites exhibits 98.8 % product yield for the oxidation of diethanolamine to iminodiacetic acid at only 30 °C. The catalyst system is further extended to the oxidation of other amino alcohols, involving monoethanolamine and triethanolamine, to their corresponding amino acids with excellent catalytic performance.

研究领域: 催化化学 · 材料科学
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CHINESE JOURNAL OF CATALYSIS · 2025 · IF 17.7

H-incorporated PdRu electrocatalyst for water splitting under alkaline condition

Hao Wu,Xian Jiang,Jingyu Lu,Yibo Li,Xinyan Li,Guidong Ju,Rengui Li,Jing Zhang

The hydrogen evolution reaction (HER) in alkaline water electrolysis faces significant kinetic and thermodynamic challenges that hinder its efficiency and scalability for sustainable hydrogen production. Herein, we employed an in-situ synthesis strategy to incorporate H atoms into the PdRu alloy lattice to form H Inc -PdRu electrocatalyst, thereby modulating its electronic structure and enhancing its alkaline HER performance. We demonstrate that the incorporation of H atoms significantly improves electrocatalytic activity, achieving a remarkably low overpotential of 25 mV at 10 mA cm –2 compared with the Pd, Ru and PdRu catalysts while maintaining robust catalyst stability. Operando spectroscopic analysis indicates that H insertion into the H Inc -PdRu electrocatalyst enhances the availability of H 2 O* at the surface, promoting water dissociation at the active sites. Theoretical calculations proposed that the co-incorporating H and Ru atoms induces s-d orbital coupling within the Pd lattices, effectively weakening hydrogen adsorption strength and optimizing the alkaline HER energetics. This work presents a facile approach for the rational design of bimetallic electrocatalysts for efficient and stable alkaline water electrolysis for renewable hydrogen production.

CAS / MDL: 100-51-6 14898-67-0
研究领域: 电催化 · 氢能 · 材料科学 · 可再生能源 · 物理化学
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Small · 2024 ·Vol. 20 ·期 26 ·2310226 · IF 13

Dual-Stimuli-Responsive Modulation Organic Afterglow Based on N─H Proton Migration Mechanism

Zhongwei Man,Zheng Lv,Yangyang Cao,Zhenzhen Xu,Qing Liao,Jiannian Yao,Feng Teng,Aiwei Tang,Hongbing Fu

Organic afterglow materials have significant applications in information security and flexible electronic devices with unique optical properties. It is vital but challenging to develop organic afterglow materials possessing controlled output with multi-stimuli-responsive capacity. Herein, dimethyl terephthalate (DTT) is introduced as a strong proton acceptor. The migration direction of N─H protons on two compounds Hs can be regulated by altering the excitation wavelength (Ex) or amine stimulation, thereby achieving dual-stimuli-responsive afterglow emission. When the Ex is below 300 nm, protons migrate to S 1-2 DTT , where strong interactions induce phosphorescent emission of Hs , resulting in afterglow behavior. Conversely, when the Ex is above 300 nm, protons interact with the S 0 DTT weakly and the afterglow disappears. In view of amine-based compounds with higher proton accepting capabilities, it can snatch proton from S 1-2 DTT and redirect the proton flow toward amine, effectively suppressing the afterglow but obtaining a new redshifted fluorescence emission with Δλ over 200 nm due to the high polarity of amine. Moreover, it is successfully demonstrated that the applications of dual-stimuli-responsive organic afterglow materials in information encryption based on the systematic excitation-wavelength-dependent (Ex-De) behavior and amine selectivity detection.

研究领域: 材料科学 · 光学材料 · 刺激响应材料 · 信息加密 · 物理化学
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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Mussel-inspired encapsulation of poly(pyrogallol-tetraethylenepentamine) resin into mesoporous MSU-H matrix and its rapid removal feature for Congo red from aquatic environment

Qiang Liu,Qiying Yang,Qiuyue Zhang,Fei Lv,Aiyuan Cheng,Hanxiao Liu,Shuanhong Ma,Likai Wang,Qinze Liu

Removing organic dyes from polluted water by mesoporous polymeric composite has recently attracted intensive attentions. Herein, the mesoporous poly(pyrogallol-tetraethylenepentamine)/MSU-H (PPTA/MSU-H) adsorbent was tapped for the capture of Congo red (CR) in aquatic environment via mussel-inspired encapsulation strategy. Many characterizations ( e.g. FT-IR, SEM, BET, etc ) are employed to confirm the successful decoration of PPTA resin. Effects of composite components, initial concentrations, environmental temperatures, adsorbent dosages, initial pH values, and foreign ions on the removal of CR by PPTA/MSU-H- x composites have been investigated successively. At optimal conditions of process variables, PPTA/MSU-H-20 exhibits the highest R % value (94.79 %) and reaches adsorption equilibrium at 180 min. The adsorption behavior of the representative adsorbent is matched well with the pseudo-second-order model, meaning one CR molecule binds with two capture sites. Furthermore, it indicates a monolayer homogeneous adsorption on PPTA/MSU-H-20 with the maximum theoretical capacity of 222 mg g −1 according to the well fitted Langmuir model. The removal mechanism of CR may be ascribed to hydrogen bonding, π-π stacking, electrostatic attraction, pore filling effects, and addition reaction. Overall, results reveal that mesoporous PPTA decorated adsorbent has a rewritable refabrication character and excellent specificity for the anionic dye purification in polluted water.

CAS / MDL: 87-66-1 112-57-2
研究领域: 环境科学 · 材料科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2017 · IF 9.446

Graphene-analogue h-BN coupled Bi-rich Bi4O5Br2 layered microspheres for enhanced visible-light photocatalytic activity and mechanism insight

Shanshan Ding,Danjun Mao,Shaogui Yang,Fei Wang,Lingjun Meng,Mengshu Han,Huan He,Cheng Sun,Bin Xu

The novel boron nitride coupled Bi-rich Bi 4 O 5 Br 2 layered microspheres (h-BN/Bi 4 O 5 Br 2 -LMs) were successfully synthesized via a facile ionic liquid-in-water (IL/W) microemulsion-mediated route. The physical, chemical and optical properties of these heterojunction photocatalysts were thoroughly characterized with X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM) equipped with energy dispersive X-ray spectrometry (EDS), transmission electron microscopy (TEM) and UV–vis diffuse reflection spectroscopy (DRS). Their photocatalytic activities were primarily evaluated by degradation of 4- tert -butylphenol (PTBP), which found 1.0   wt% h-BN/Bi 4 O 5 Br 2 -LMs to be the best one. The photocurrent experiments showed that the photocurrent density of 1.0   wt% h-BN/Bi 4 O 5 Br 2 -LMs was four times higher than that of pure Bi 4 O 5 Br 2 -LMs due to enhanced charge transfer ability of the former. It revealed that the addition of h-BN was in favor of suppressing the photoinduced electron-hole pair recombination of Bi 4 O 5 Br 2 -LMs, so as to improve the photocatalytic activity of the composite. O 2 − and h + were proved to be the main reactive species in the photocatalytic process by scavenger experiments and electron paramagnetic resonance (EPR) spectra. In addition, the photocatalytic mechanism of h-BN/Bi 4 O 5 Br 2 -LMs was further elaborated in this work. The probable degradation products were identified by GC–MS. The proposed conjugated addition and oxidation reactions were described to be the main pathways by combining the frontier electron density calculation and GC–MS results.

研究领域: 材料科学 · 环境科学 · 化学工程
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JOURNAL OF ORGANIC CHEMISTRY · 2023 · IF 3.6

Selective Oxidative Methyl C–H Functionalization of Butylated Hydroxytoluene toward Arylimines/N-Heterocycles

Jianyu Dong,Shaofeng Wu,Furong Geng,Yani Yan,Long Liu,Yongbo Zhou

A metal-free and selective oxidative methyl C–H functionalization of BHT with aniline compounds has been developed. This innovative method enables the facile and efficient synthesis of a diverse array of BHT-functionalized N-containing skeletons, including arylamines, benzoxazoles, benzothiazoles, benzimidazoles, quinazolines, and quinazolinones, all of which are challenging to access. The control experiment involving TEMP18O suggests that the radical adduct of TEMPO with the benzyl radical of BHT may serve as an intermediate.

研究领域: 有机化学 · 合成化学
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