ACS Applied Energy Materials
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2022
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IF 6.959
Yan Zhang,Chuang Chen,Qiu-Hui Zheng,Zhan-Kuo Guo,Bao-Xia Dong,Yun-Lei Teng
Metal heteroatom doped carbon materials display remarkable catalytic performance in the electrochemical CO2 reduction (ECR) because the doped heteroatoms can significantly change the local density of state and electronic structure of carbon, which induces charge polarization or structural defects. Herein, we synthesized S-doped NiII-triazolate precursors with high purity and crystallinity through a simple one-step hydrothermal method. The high-temperature pyrolysis process produced a series of Ni–S–CT (T = 800, 900, 1000 °C) materials with Ni3S2 as the main component. It resulted in significant carbon structure defects in the catalyst, which increased the specific surface area and pore volume, providing a basis for improving the ECR activity. Through the structural characterizations of powder X-ray diffraction (PXRD), Raman, X-ray photoelectron (XPS), Brunauer–Emmett–Teller (BET), transmission electron microscopy (TEM), and electrochemical characterizations of linear sweep voltammetry (LSV), chronoamperometry (i–t curve), electrochemical impedance spectroscopy (EIS), and electrochemical active surface area (ECSA), as well as gaseous product analysis, we can build the structural-performance relationship. Ni–S–CT catalysts all reached the highest CO Faraday efficiency at −1.5 V vs Ag/AgCl potential, among which Ni–S–C1000 exhibited the best catalytic activity (FECO of 66.6% and jCO of 1.28 mA/cm2). It also displayed excellent stability and recyclability, which could realize the efficient reuse of the catalyst. In addition, the density functional theory (DFT) calculation was carried out on Ni3S2 to illustrate the ECR activity origination. It is the first report on Ni3S2-based catalysts in the application of ECR.
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CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Tong Liu,Zhican Xie,Peng Zhou,Zhaokun Xiong,Heng Zhang,Zhicheng Pan,Yang Liu,Bo Lai
Transition metal activation of sulfite (S(IV)) is a promising wastewater treatment technology . In this study, the activation of potassium pyrosulfite (PPS) with ferric iron (Fe 3+ ) is proposed firstly to degrade carbamazepine (CBZ). PPS has the advantages of low cost, non-toxicity and acidic solution, which makes it unnecessary to adjust the pH. The results showed that the Fe 3+ cycle was realized during the reaction process, and the degradation trend of CBZ was consistent with the formation rate of Fe 2+ and the decay rate of S(IV). Moreover, oxygen (O 2 ) plays a decisive role in the system and was the initiator of free radical chain reactions. The existence of sulfite radical (SO 3 •− ), sulfate radical (SO 4 •− ) and hydroxyl radicals (HO • ) in Fe 3+ /PPS system was proved by electron paramagnetic resonance (EPR), quenching experiments and terephthalic acid (TA) photoluminescence probing technique. The contribution of SO 4 •− and OH • to the removal of CBZ in Fe 3+ /PPS system is 64% and 35%, respectively. In addition, intermediates of CBZ were identified by Liquid Chromatography–Tandem Mass Spectrometry (LC–MS/MS) and possible removal pathways were also proposed. Finally, the effects of PPS concentration, Fe 3+ concentration, initial pH, anions and humic acid (HA) were also investigated.
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SOLAR ENERGY MATERIALS AND SOLAR CELLS
·
2017
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IF 4.784
Shoushuai Gao,Yi Zhang,Jianping Ao,Shuping Lin,Zhaojing Zhang,Xiuling Li,Dongxiao Wang,Zhiqiang Zhou,Guozhong Sun,Fangfang Liu,Yun Sun
The direction of Se-Mo-Se sheets to the Mo film is crucial for the thickness of Mo(S,Se) 2 and the electrical conductivity , so as the back contact of Cu 2 ZnSn(S,Se) 4 solar cells. In this study, the preferred orientation of Mo(S,Se) 2 film changes from (100) peak to (103) peak, i.e. from perpendicular to the substrate to tilted to the substrate for Se-Mo-Se sheets as the roughness decrease of Mo back contact layer. The Se vapor can easily diffuse through the channels between Se-Mo-Se sheets when the formed Mo(S,Se) 2 layer is (100) peak preferred with Se-Mo-Se sheets perpendicular to the substrate, and thus excessively thick Mo(S,Se) 2 will be formed. Whereas, the Se-Mo-Se sheets are tilted to substrate when the preferred orientation of Mo(S,Se) 2 is (103) peak. The tilted Se-Mo-Se sheets can act as a natural Se diffusion barrier to suppress the Se vapor diffusion through the already formed Mo(S,Se) 2 layer to further selenize the remaining Mo film, and also can provide a good electrical conductivity. As a result, the thickness of Mo(S,Se) 2 sharply decreased from 1500 nm to 200 nm with the surface morphology change of Mo back contact, which resulting in the decrease of series resistance of Cu 2 ZnSn(S,Se) 4 solar cells from 2.94 Ω cm 2 to 0.49 Ω cm 2 , and the increase of conversion efficiency of Cu 2 ZnSn(S,Se) 4 solar cells from 6.98% to 9.04%.
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INORGANIC CHEMISTRY
·
2024
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IF 4.3
Minglun Cheng,Sibo Shen,Zhiwei Zhang,Kui Niu,Ning Wang
Electroreduction of CO2 to value-added low-carbon chemicals is a promising way for carbon neutrality and CO2 utilization. It was found that the diiron complex [(μ-bdt)Fe2(CO)6] (bdt = benzene-1,2-dithiolate) has high catalytic activity for electrocatalytic CO2 reduction. To further study the effect of the S-to-S bridge on the catalytic performances of diiron complexes for electrochemical CO2 reduction, four diiron complexes 1–4 with different rigid and conjugated S-to-S bridges were either selected or designed. The electrocatalytic studies showed that under optimal conditions, 2 with a 2,3-naphthalenedithiolato bridge exhibited the lowest catalytic onset potential (Eonset = −1.75 V vs Fc+/0), while 4 with a diphenyl-1,2-vinylidene bridge displayed the highest catalytic activity (TOFmax = 295 s–1), which is 1.5 times that of [(μ-bdt)Fe2(CO)6]. The controlled potential electrolysis experiments of 4 in 0.1 M MeOH/MeCN at −2.35 V vs Fc+/0 gave a total faradaic yield close to 100%, with selectivities of 77%, 9%, and 14% for HCOOH, CO, and H2, respectively. The mechanism for CO2 reduction was studied using density functional theory, IR spectroelectrochemistry, and electrochemical methods. The results indicate that modifying the structure of the S-to-S bridge is an effective strategy to improve the catalytic performance of diiron complexes for electrocatalytic CO2 reduction.
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PubMed
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2024
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IF 5.3
Chenlu Chen,Yue Xu,Zhiruo Li,Yinxin Yang,Yuxu Tao,Xiaoxuan Wang,Yini Wang,Haikuan Yuan,Lijuan Zhang,Xijian Liu,Jie Lu
In this article, the molar fraction solubility of (R,S)- and (S)-tetramisole hydrochloride in two binary solvents (methanol + ethanol and methanol + toluene) was measured by experiments between 283.15 K and 323.15 K. Then four different equations including Apelblat equation, λh equation, GSM equation, Jouyban-Acree equation were applied to connect the measured solubility data of (R,S)- and (S)-tetramisole hydrochloride, where Apelblat equation had the minimum ARD %. The crystal structures together with intermolecular interactions of (R,S)- and (S)-tetramisole hydrochloride were then analyzed. In addition, the infrared spectra were also simulated using dimer configurations. Furthermore, molecular dynamic simulations including radial distribution function (RDF) combined with solvation free energy were performed to explore solvent–solvent interactions along with solute–solvent interactions. The results showed that there was co-solvency in methanol + toluene binary solvent. According to simulation results, both solvent–solvent interactions and solute–solvent interactions played an important role in affecting the solubilities of (R,S)- and (S)-tetramisole hydrochloride. In the end, combining solid state characterization and ternary phase diagrams, (R,S)-tetramisole hydrochloride was determined to be a racemic compound. All the results in this paper can provide theoretical support for enhancing crystallization resolution techniques for chiral drugs.
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INORGANIC CHEMISTRY
·
2019
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IF 4.85
Shikang Yin,Jinze Li,Linlin Sun,Xin Li,Dong Shen,Xianghai Song,Pengwei Huo,Huiqin Wang,Yongsheng Yan
Photocatalytic reduction of CO2 by semiconductors is of great significance in generating value-added fuels. Here, we construct a novel S–C–S heterojunction constituted of MoS2/SnS2/r-GO by a simple solvothermal method. The prepared MoS2/SnS2/r-GO showed significant photoexcitation of photosensitive oxygen (ROS) by electron spin resonance spectroscopy, demonstrating that superoxide radicals (•O2–), pores, and hydroxyl radicals (•OH) are the main active species. The constructed S–C–S heterojunction has a multilevel electron transport mechanism and synergistic effect, which provides the possibility of producing more organic fuel. The photocatalytic materials were characterized by XRD, XPS, SEM, TEM, PL, etc. As a result, the atomic layer MoS2/SnS2/r-GO heterojunction exhibited a CO formation rate of 68.53 μmol g–1 h–1 and a CH4 formation rate of 50.55 μmol g–1 h–1, respectively. This work opens up new prospects for the formation of heterojunctions of chalcogenide transition-metal sulfides.
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Molecular Catalysis
·
2026
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IF 4.3
Qi Li,Qi Zhang,Feng Wang
Conjugated porous polymers (CPPs) represent a novel class of photocatalysts for hydrogen peroxide (H 2 O 2 ) production. Their photocatalytic activity can be enhanced through rational design of the electronic structures. Herein, three donor–acceptor (D–A) type CPPs with expanded saddle-shaped structures were constructed by copolymerizing dibenzothiophene-S,S-dioxide with different electron donating units, including triphenylamine, 1,3,5-triphenylbenzene, and 2,4,6-triphenyltriazine. Among the prepared CPPs, the dibenzothiophene-S,S-dioxide-triazine-based polymer shows impressive photocatalytic H 2 O 2 production rate of 2.98 mmol g −1 h −1 under the optimal condition, which is among the top photocatalytic performance reported so far for the existing CPPs. Experimental and theoretical studies revealed that the introduction of triazine linkages not only prolongs carrier lifetime and increases charge separation efficiency, but also reduces the energy barrier for O 2 activation. This study elucidates that rational design of dibenzothiophene-S,S-dioxide-based photocatalysts by tailoring electron-donating strength, charge transfer orientation and O 2 adsorption sites is crucial for efficient H 2 O 2 production.
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ACS Applied Polymer Materials
·
2026
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IF 5.2
Wenbo Luan,Xiaodong Sui,Xiaoling Jian,Like Chang,Jiawei Xu,Longhai Guo,Teng Qiu,Jun Ye,Xinlin Tuo
The inherent trade-off among colloidal stability, reliable mechanical performance under thermal and thermo-oxidative aging, and reprocessability remains a critical bottleneck limiting the broader technological application of waterborne polyurethanes (WPU). Herein, inspired by the concepts of biomimetic artificial foldamers and reversible covalent cross-linking, we demonstrate an WPU system characterized by the synergism of a rigid poly(p-phenylene sulfone amide) based physical network and flexible thioctic acid (TA)-based dynamic S–S network. The strong interactions between PSA segments contribute to ordered H-bonding and π–π stacking, and the sulfone groups contribute to the improved thermal stability and the copolymerization compatibility with WPU. The TA linkages function as supplementary cross-linking and antioxidants, and their flexibility and metathesis reactions provide the kinetic possibility for the adjustment and rearrangement of the PSA network. Well-dispersed dispersion was constructed and produced an excellent elastomer by film formation. In comparison with the controlled blank sample, the dual network exhibited an increase on the tensile strength of 2.4 folds at room temperature, 67 folds at a high temperature of 120 °C, 7.2 folds after 7 days of aging at 120 °C, and 25 folds after three times of reprocessing by thermal pressing. The relatively high elongation at break and good toughness were also largely maintained under all the conditions. The heat deflection temperature increased by 133 °C. The rigid–flexible dual-network WPU, featuring unique environmental friendliness, operation feasibility together with unique thermal robustness, mechanical adaptability, and dynamic network reconfiguration capability represents an effective material platform for the potential high-end use such as high-temperature flexible electronics, stress-buffering components, and reconfigurable elastomeric structures.
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EUROPEAN POLYMER JOURNAL
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2026
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IF 6.8
Mengchao Zhang,Bingbing Guo,Sifan Li,Jing Chen,Hongkun Li
Alkyne polycyclotrimerization has emerged as a versatile synthetic platform for the preparation of hyperbranched polyphenylenes. However, most existing systems rely on transition metal catalysts, suffer from harsh reaction conditions, and yield regioirregular polymers, which limit their practical applicability. Herein, we present a facile and efficient strategy for the synthesis of regioregular hyperbranched polymers via organocatalyzed polycyclotrimerization of activated terminal diynes. Specifically, the polymerization reactions of bis(aroylacetylene)s were conducted in dichloromethane (DCM) at 30 °C for 5 h in the presence of 4-dimethylaminopyridine (DMAP) and acetylacetone, affording five soluble hyperbranched poly(aroylarylene)s ( hb -PAAs) with high weight-average molecular weights of up to 1251000 g/mol in high yields of up to 90.7%. Notably, the polycyclotrimerization proceeds smoothly under open-air conditions without the need for moisture or oxygen exclusion. The hb -PAAs possess perfect 1,3,5-regiostructures, and high thermal stabilities with 5% weight loss temperatures up to 482 °C. The hb -PAA incorporating tetraarylethylene (TAE) moieties exhibits distinct aggregation-induced emission (AIE) characteristics. Furthermore, when doped into a poly(vinyl alcohol) (PVA) matrix, the polymers display room-temperature phosphorescence (RTP) properties, with phosphorescence lifetimes of up to 320 ms and phosphorescence quantum yields ( Φ p ) of up to 4.8%. This organocatalytic polycyclotrimerization provides a mild, metal-free route to regioregular hyperbranched polymers with tailored photophysical properties, showing great potential for advanced optoelectronic applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
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IF 6.371
Dong Gao,Xiao Ji,Hongwei Yu,Zhanggui Hu,Jiyang Wang,Yicheng Wu,Hongping Wu
Four new metal chalcogenides containing fluorine, Na 2 Ba 17 In 8 Q 21 F 18 (Q = S, Se), KBa 2 InQ 3 F 2 (Q = S, Se) were synthesized by the solid-state reactions, and their structures were determined by single crystal X-ray diffraction. To the best of our knowledge, they represent the first example of F-containing mixed alkali and alkaline earth In-based chalcogenides . Structurally, Na 2 Ba 17 In 8 Q 21 F 18 (Q = S, Se), KBa 2 InQ 3 F 2 (Q = S, Se) all feature one-dimensional chain-like structures composed of In-based polyhedra, but they are not isostructural. The optical property measurements indicate that KBa 2 InSe 3 F 2 and Na 2 Ba 17 In 8 Se 21 F 18 have relatively large birefringences (0.096 and 0.083 at 532 nm, respectively), which are larger than that of KBa 2 InS 3 F 2 (0.056 @ 532 nm) and Na 2 Ba 17 In 8 S 21 F 18 (0.041 @ 532 nm). Their structure-property relationship demonstrates that the large difference of birefringence among these compounds mainly arises from the different connection modes of InQ n (n = 4, 5) polyhedra. In addition, the first-principles calculations, UV–vis–NIR diffuse reflectance spectra and IR spectroscopy of title compounds have also been performed. The effect of M III /cation ratios on the polymerization of In–Q (Q=S, Se) units have been discussed.
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HIGH PERFORMANCE POLYMERS
·
2015
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IF 1.286
Jiangtao Liu,Guofei Chen,Xingzhong Fang
A series of isomeric poly(thioether imide)s (PTIs) containing thioether linkages were prepared by aromatic nucleophilic substitution reaction of isomeric bis(chlorophthalimide)s (BCPIs) and bisthiophenols. The glass transition temperatures (Tgs) of the isomeric PTIs were 190–264°C, the 5% weight loss temperature (T5%) reached up to 441–508°C under nitrogen and 472–520°C in air atmospheres, respectively. It was found that the Tg values of the PTIs from three isomeric BCPIs with the same bisthiophenol increased in the order of 4,4′-BCPI < 3,4′-BCPI < 3,3′-BCPI, while the T5% values gradually decreased in the order of 4,4′-BCPI > 3,4′-BCPI > 3,3′-BCPI. Flexible films that could be cast from the polymer solutions exhibited good mechanical properties with tensile strengths of 91–121 MPa, elongations at break of 8–12%, and tensile moduli of 2.2–2.6 GPa. The minimum melt viscosity of isomeric PTIs decreased with increasing the content of asymmetric 3,4′-substituted phthalimide unit, and the PTI (2c) showed the lowest melt viscosity about 760 Pa·s at 264°C among these isomeric polymers.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2024
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IF 4.9
Worku Lakew Kebede,Dong-Hau Kuo,Xiaoyun Chen
Environment and energy are presently some of the highest priority topics for mankind that need to be addressed. Organic pollutants are toxic and carcinogenic for human and aquatic life hence their presence in water even in low concentrations can cause serious health problems. Photodegradation of organic pollutants by utilizing oxide-based heterostructure photocatalysts is the promising approach to carry out remediation efficiently ascribed to the advanced optoelectronic and structural superiority of oxide photocatalysts. The Zn(O,S)/Mo(O,S) 2 composites were synthesized via a facile solvothermal method at low temperatures. Several methods were used to characterize the composite morphology, structure, electrical conductivity, chemical composition, and optical characteristics. The heterostructured Zn(O,S)/Mo(O,S) 2 oxysulfide was employed successfully in the photocatalytic degradation of organic pollutants. Among the as-prepared samples, the 30-ZnMoOS composite catalyst was found to have the highest photodegradation performance on various organic dye pollutants. The photocatalytic activity of the as-synthesized Zn(O,S)/Mo(O,S) 2 samples was assessed on the photodegradation of different kinds of organic dyes under visible light irradiation. The photocatalytic degradation efficiency of 30-ZnMoOS composite over 10 ppm neutral red (NR), methylene blue (MB), rhodamine B (Rh B), and methyl orange (MO) was found to be 99.6 %, 99.9 %, 99.5 %, and 98.8 % within 40, 45, 180, and 180 min, respectively, under visible light illumination. In the present photocatalytic system, the superoxide ( . O 2 - ) anions, hydroxyl ( . OH) radicals, and holes (h + ) are proposed to be the direct reactive species causing the photodegradation of organic dyes.
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