Surfaces and Interfaces
·
2023
·
IF 6.2
Tingyu Chen,Shuaiqi Zhao,Jiajin Lin,Yanan Chong,Yifei Li,Yun Zhao,Guangxu Chen,Yongcai Qiu
As a nontoxic and cheap catalyst, the Al 2 O 3 catalyst can be used to catalyze the propane dehydrogenation (PDH) process. However, due to its poor activity, it has been used as a catalyst carrier rather than catalysis. In this work, the experimental results indicate that γ- Al 2 O 3 -(110)-S catalysts can improve the yield of propane dehydrogenation more effectively than γ-Al 2 O 3 -(110) catalyst. We investigate the potential barrier of propane dehydrogenation reaction catalyzed by Al 2 O 3 -(110) under different conditions and found that the substitution of the S atom for partial O atom can modify the acid-base properties of the surface active site of γ-Al 2 O 3 -(110), thus reducing the reaction energy barrier. In particular, the yield of the reaction can be further improved by the active sites of oxygen vacancies generated by removing partial S atoms in γ-Al 2 O 3 -(110)-S, which is consistent with our theoretical calculation results. At the same time, theoretical calculation shows that Cu clusters can effectively remove the S atoms on the surface of γ-Al 2 O 3 -(110)-S and form oxygen vacancies. This strategy provides a new path to form oxygen vacancies on γ-Al 2 O 3 -(110), which opens up a new way for the study of propane dehydrogenation.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Ruotong Cui,Wenlong Xu,Yanpeng Zhang,Jingxian Wang,Yingyun Qiao,Yuanyu Tian
Identifying and analyzing the reaction process of S atoms in coal at the molecular level has been a key and difficult problem in coal chemistry. Here, we used dibenzyl sulfide as a model compound for S-containing substances in coal and predicted the pyrolysis process of C-S in coal through the pyrolysis products, which indicated that the C-S bond would be broken firstly above the energetic basis point to generate intermediate S-containing radicals. A hydrogen-donating solvent (9, 10-dihydroanthracene) was utilized as the radical trapping agent to reveal the S-containing radical reaction process through the changes of the products before and after the trapping reaction. Density functional theory was further used to calculate the pyrolysis process to help verify the radical history of the response. Finally, pyrolysis experiments were performed on raw coal to confirm the generality of the pyrolytic radical regulatory mechanism of C-S. This study identifies and analyzes the relationship between C-S structure and reactivity during coal pyrolysis at the molecular level, and confirms the universal law of raw coal’s pyrolytic radical reaction mechanism. This not only provides theoretical guidance and a basis for the free radical regulation process during the pyrolysis of S-containing structures in coal but also provides theoretical support for the clean and efficient utilization of coal.
研究领域:
煤炭化学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
EUROPEAN POLYMER JOURNAL
·
2024
·
IF 5.8
Shi-Si Li,Jun-Lin Pan,Xi-Long Chen,Jing Xu,Zi-Long Li,Chunzu Cheng
Long-chain aliphatic polyesters are recognized as the most promising polyethylene mimics in that these materials show comparative physicochemical properties to polyolefins and own the unique merits of degradability and/or recyclability. Nevertheless, the application scenarios of these polymers are rather limited owing to the lack of functional groups. Herein, sulfur atoms are incorporated into the microstructures of long-chain aliphatic polyesters to decipher the variations of physicochemical properties upon replacing specific methylene units by thioether moieties and simultaneously impart polyethylene-like materials with functionalities. First of all, high molecular weight polyesters P1 - P4 and poly(β-thioester)s P5 - P8 were obtained via condensation polymerization and thiol-Michael polyaddition, respectively. As for phase transition behaviors, poly(β-thioester)s show inferior crystallization/melting temperatures and the corresponding enthalpy changes than their polyester counterparts, and a loosely packed crystalline structure should be responsible for such thermal property degradation. It is reasonable that replacing specific methylene units of long-chain aliphatic polyesters by sulfur atoms, the much bulkier functional entities, will definitely cause great disturbance to the regular arrangement of polymer chains. The rapid hydrolytic degradation of poly(β-thioester)s in acidic and alkaline media can be ascribed to the easy penetration of water molecules into their incompact amorphous/crystalline regions. In the meantime, these poly(β-thioester)s exhibit great prospects in noble metal recovery and information encryption (optical anticounterfeiting). For instance, poly(β-thioester) P5 is an excellent adsorbent to abstract gold ions from water due to its outstanding metal coordination capability. Moreover, poly(β-thioester) P5 emits bright blue photoluminescence in concentrated solution and solid state upon UV irradiation as a result of the clustering-triggered through space electron delocalization and rigidified polymer chain conformation.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
DYES AND PIGMENTS
·
2025
·
IF 4.2
Junhong Liang,Xudong Li,Furong Shi,Jinye He,Sheng Guan,Yuan Zhou,Pengzhi Guo,Chenglong Wang,Yangjun Xia
Continuous interpenetrating network morphology on the performance of organic solar cells (OSCs) have the effect of ease, how to control the bulk heterojunction (BHJ) the formation of the fiber morphology is of vital importance. In this study, a series of polymers were synthesized by rationally varying the atoms connecting the conjugated backbone and side chains, PBDT-T-SBDD, PBDT-TS-SBDD and PBDT-TDS-SBDD were used to systematically study the effects of sulfur atom on the electron conformation of the molecule, the morphology of the blend film and the properties of the device. We found that the introduction of sulfur atoms can enhance the intermolecular interaction, thus reducing the energy disorder of the blend film. However, excessive introduction of sulfur atoms leads to excessive steric hindrance of side chain of the molecules, resulting in excessive local aggregation. Compared with PBDT-T-SBDD: Y6 and PBDT-TDS-SBDD: Y6-based OSCs, PBDT-TS-SBDD: Y6-based OSCs has both higher photovoltaic performance, reaching a PCE of 11.33 %, due to the well-defined fiber structure which significantly improves the charge transport channel and phase separation of the blend film.
研究领域:
材料科学
·
能源科学
✓ 已验证
DOI
高影响因子
ACS Applied Polymer Materials
·
2023
·
IF 5
Zhao-Bo Hou,Wei-Lin Xie,Gui-Xiang Liu,Shuangquan Liao,Ming-Chao Luo
Sulfur cross-linking, known as vulcanization, is an extraordinarily important process to endow rubbers with practical performances in the rubber industry. However, the steric hindrance of vulcanization intermediates hinders the formation of vulcanization networks, limiting the property enhancement of vulcanized rubbers. To promote the formation of vulcanization networks, our group lowers the steric hindrance of vulcanization intermediates through decreasing the length of alkyl chain. Temperature-dependent Fourier transform infrared spectroscopy suggests the formation of bridging bidentate zinc/fatty acid salt complex (vulcanization intermediates) with different steric hindrances. The reduction in steric hindrance of vulcanization intermediates increases the coordination interactions between sulfur and vulcanization intermediates, promoting the ring-opening of sulfur and formation of vulcanization networks. As a result, with the reduction in steric hindrance of vulcanization intermediates, the properties of vulcanized rubbers improve greatly. This work promotes the formation of vulcanization network through lowering the steric hindrance of vulcanization intermediates, which provides a simple generic strategy for the development of high-performance rubbers.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2022
·
IF 6.14
Wanying Lin,Biao Zhang,Jun Jiang,Enzuo Liu,Junwei Sha,Liying Ma
The design of transition metal dichalcogenides that satisfies the essential requirements of the hydrogen evolution reaction (HER) in alkaline solutions remains a challenge. The study gives a description of sulfur atoms into both anionic and cationic sites of WTe2, which is deliberately designed and has been rarely reported. Herein, we report 3D self-supported anionic and cationic S-substituted WTe2 nanosheet arrays constructed on a carbon cloth by a three-step synthesis method at elevated temperatures. Experimental and theoretical analysis are both executed to investigate S-WTe2/CC nanocomposites for efficient alkaline HER, and the results attest to its excellent electrocatalytic performance. The optimized S-WTe2/CC exhibits an enhanced HER activity with an overpotential of 195 mV at the current density of 10 mA cm–2, which is 2.3 and 1.7 times lower than that of WO3/CC (451 mV) and WTe2/CC (327 mV), respectively. According to density functional theory calculations, such improvement of alkaline HER is attributed to the optimized p-band electron configuration of Te atoms, higher H* intermediate adsorption, and lower H2O dissociation energy barrier by anionic and cationic co-substitution of S, which accelerate the Volmer–Heyrovsky process. The present study paves a way to the modification strategy of WTe2 electrocatalysts.
研究领域:
材料科学
·
电化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Chao Hu,Huimin Qi,Jingfu Song,Gai Zhao,Jiaxin Yu,Yafeng Zhang,Hongtu He,Jianping Lai
In order to explore the friction and wear mechanisms of polyimide with metal, this work addressed the tribological properties of the polyimide with different molecular structures in a wide temperature range. It was found that the incorporation of fluorine and sulfur atoms into polyimide had a significant effect on their mechanical and tribological properties. Generally, the wear rates of FPI and SPI are much higher than PI, and FPI displays the worst friction coefficient. To deeper reveal the fundamental reasons, the FTIR, XPS, EDS, SEM characterizations were carried out combined with molecular dynamic simulation. The calculation results from the Molecular Dynamics model between PI and Fe showed that the interaction potential energy of SPI and FPI was larger than that of PI due to the polarization of F and S. Judged from the structures of transfer film, SPI and FPI was easily adhered on the surface of counterpart, even chemical reaction. The XPS analysis further confirmed the possibility of tribo-chemical reactions between SPI/FPI and Fe. This study will provide the theoretical guidance for other polymer molecular design and its tribological research.
研究领域:
材料科学
·
摩擦学
✓ 已验证
产品关联
DOI
高影响因子
LETTERS IN ORGANIC CHEMISTRY
·
2023
·Vol. 20
·期 12
·1159-1169
·
IF 0.8
Yaghoubi Fatemeh,imanzadeh Gholamhassan,Asgharzadeh Roghayyeh,Soltanzadeh Zahra,Öztürk Turan
Dihydropyrimidines are one of the most important heterocyclic ring systems having a serious place in medicinal and organic synthesis. In this paper, a new series of dihydropyrimidines consisting of sulfur atoms were synthesized using inorganic base K2CO3 and TBAB as an organic salt
to make high polarity in reaction media. Interestingly, different 3,4-dihydropyrimidin-2(1H)-thiones reacted smoothly with various acrylic esters to afford adducts viahighly regioselective N3-Michael addition reaction was carried out at 100°C in 12 h. result: Unfortunately, the
reaction failed with fumaric esters owing steric effects. Avoiding organic solvents during this reaction effectively led to the development of an economic approach. Structures of the new compounds were established on the basis of 1H NMR, 13C NMR, and IR spectral data.
研究领域:
有机化学
·
药物化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Qi Xu,Song Wang,Yuntao Wang,Xiankun Wu,Jingtao Dai,Jianlan Liu,Dong Fang,Cheng Zhang,Shixin Sun,Tao Cheng,Hao Yang,Guodong Xu,XiaoMing Ren,Jiahui Kou
The utilization of carbon nitride (C 3 N 4 ) in photocatalytic CO 2 reduction faces obstacles due to significant charge recombination of photogenerated electron-hole pairs, limited light-harvesting capability, and a constrained surface area. In this study, S-C 3 N 4 /IL composites were synthesized by molecular docking of ionic liquids (IL) through S atoms in layered carbon nitride under environmental conditions by simple self-assembly technology to achieve efficient photocatalytic CO 2 reduction. Contrasted with pristine C 3 N 4 (1.1 μmol g -1 h −1 ), S-C 3 N 4 /IL demonstrated over a 300-fold increase in the rate of CO 2 reduction to CO (310 µmol g -1 h −1 ), achieving an approximate 100 % selectivity. Moreover, the possible reaction mechanism was proposed by in-situ infrared and DFT calculations. The remarkable photocatalytic efficacy of S-C 3 N 4 /IL can be ascribed to multiple factors: 1) augmented visible light absorption range and enhanced interfacial compatibility due to sulfur doping, fostering improved interaction between the amphiphilic ionic liquid and the hydrophobic C 3 N 4 ; 2) suppressed char + ge recombination, facilitating increased generation of abundant free radicals; 3) the Coulombic interaction between the IL’s anionic and cationic components with the formed electron-hole pairs, thereby impeding their recombination. Besides, ultraviolet photoelectron spectroscopy, fluorescence lifetime support these results. DFT calculation suggests S doping also plays a critical role in reducing free energy of *COOH formation. In addition, 13 C isotope experiment confirms the carbon source of CO from CO 2 . This proposition paves the way for enhancing the photocatalytic prowess of carbon nitride in CO 2 reduction.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Yunchao Ma,Yuxin Yao,Shengnan Qi,Chuanxue You,Yuanyuan Wu,Chunbo Liu,Bo Hu,Keyu Cui
Herein, we successfully synthesized two photoactive donor–acceptor (D-A) covalent organic frameworks by incorporating electric-deficient triazine and electric-rich benzotrithiophene moieties into the framework. The introduction of sulfur atom and triazine unit significantly change the intrinsic band gap of JLNU-COFs, this leads to an expanded range of light absorption, encompassing wavelengths from ultraviolet to visible. The narrow band gap of JLNU-311 allows for efficient utilization of visible light while maintaining the thermodynamic activity required for nitrogen reduction within appropriate energy bands. JLNU-311 modified with strong electron absorbing groups has higher activity to NH 3 production without co-catalyst or sacrificial agent, and yield can reach 325.6 µmol/g/h. Theoretical calculation further confirm that acceptor structure can effectively regulate the band gap width, promote the adsorption, dissociation and protonation of N 2 molecules on JLNU-COFs, and thus reduce the energy barrier of photocatalytic nitrogen reduction reaction (PNRR). Therefore, this study provides an effective strategy for design of active nitrogen fixing photocatalysts.
研究领域:
材料科学
·
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2023
·Vol. 39
·期 5
·790-796
·
IF 3.1
Khan Munir Ullah,Khan Safir Ullah,Cao Xiaohan,Usman Muhammad,Shah Muhammad Naeem,Ghaffar Abdul,Hassan Muhammad,Zhang Chengjian,Zhang Xinghong
I n this study, we report that Berlin Green (FeFe-BG) framework exhibits superior performance in the catalytic coupling of carbon disulfide (CS 2 ) and propylene oxide (PO) to generate a random copolymer containing thioether, propylene monothiocarbonate and ether units. Oxygen and sulfur atom exchange was detected in polymeric and cyclic thiocarbonate byproducts and utilized to modulate the copolymerization of CS 2 and propylene oxide. The coupling of PO and CS 2 was selective for copolymer formation under various reaction conditions. 1 H and 13 C NMR spectroscopy determined two distinct polymer linkages and two cyclic byproducts. Copolymer number average molecular weights ranged from 6.4 kg/mol to 10.5 kg/mol, with a comparatively low polydispersity of 1.3–1.7. The CS 2 /PO molar feed ratio had a significant impact on the O/S exchange process; the ratio of cyclic thiocarbonate byproducts could be efficiently regulated by tuning the CS 2 molar feed ratio.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 9
·1-9
·
IF 5.833
Pan
Fei,Tong
Chunyi,Wang Zhaoyang,Han Haitao,Liu Pei,Pan Dawei,Zhu Rilong
An electrochemical sensor constructed by intercalated composites was developed for determination of heavy metal ions. The intercalated composites were composed of hydrosulphonyl functional covalent organic frameworks (COF-SH) and graphene (G). The presence of numerous adsorption sites, such as 18 sulfur atoms and 30 nitrogen atoms per big circle of COFs on COF-SH, was beneficial for the accumulation of heavy metals, while the graphene enhanced the electrical conductivity. The obtained sensor under the optimal conditions successfully detected the presence of heavy metal ions in coastal water samples at concentrations ranging from 1 to 1000 μg L −1 . The detection limits of Cd (II), Pb (II), Cu (II), and Hg (II) were 0.3, 0.2, 0.2, and 1.1 μg L −1 , respectively. Furthermore, the sensor still exhibited good stability after multiple uses less than 5%. When it is used in the analysis of actual samples, the recovery of standard addition is higher than 95%. In sum, the combination of hydrosulphonyl functional COFs with graphene looks very promising for the assembly of sensors with high sensitivity toward the determination of heavy metal ions for coastal environmental monitoring. Graphical abstract
研究领域:
材料科学
·
环境科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）