COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Xin Ge,Weili Song,Xinzhi Chen,Chao Qian,Shaodong Zhou,Xuemin Liu
A tandem process of micellar catalysis and cloud point extraction (CPE) is developed for copper-catalyzed Ullmann C-S coupling reactions in water. The functional nonionic surfactant, amine terminated polyether M2070, affords nano-micelle environment in the aqueous system; the latter splits to two phases above the cloud point temperature (CPT). The nature of the micellar catalysis in M2070 aqueous was investigated by DLS, EDS, XPS, IR, TEM and 1 H NMR. M2070 was verified to provide nano-space for encapsulation and aggregation of the substrates. More importantly, the metallic micelle formed by M2070 chelating copper was identified. It is noteworthy that excellent productivity in pre-micellar catalysis of C-S coupling reactions was obtained with good tolerance of substrate. Finally, the water-micelle system was separated into two phases above the CPT thus to achieve the product separation. Furthermore, the M2070/water system can be recycled and reused.
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Green Energy & Environment
·
2021
·
IF 8.207
Dashui Yuan,Zongyuan Li,Xueru Chen,Jing Ding,Hui Wan,Guofeng Guan
Proper interface and band alignment always play essential roles in the separation of photoexcited charge of photocatalysts. In this work, we prepared a homodispersed S-scheme carbon nitride homojunction with local electron structure difference by a facile pre-doping and two-step calcination approach. Boron doping into heptazine created extra acceptor impurity, and phosphorus doping into heptazine created extra donor impurity, which eventually modulated the electronic structure of carbon nitride. As heptazines with different element doping were integrated into carbon nitride by recalcination, B–CN and P–CN formed a homodispersed homojunction and thus produced a rich interface. Meanwhile, caused by Fermi energy levels equilibrium, the band bending constructed an S-scheme homojunction, which stimulated photogenerated electrons to transfer from CB of B–CN to VB of P–CN. The homodispersed S-scheme homojunction structure led to efficient suppression of recombination of photoinduced charge and retained stronger redox charge. Consequently, the photocatalytic performance was dramatically boosted to 2620 μmol g −1 from 60 μmol g −1 of pure CN in 4-h hydrogen evolution from water. This novel method for electron structure engineering helped to provide a new strategy for designing homojunction photocatalysts with excellent photocatalytic performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Junnan Tao,Xiaohui Yu,Qinqin Liu,Guiwu Liu,Hua Tang
The requisite interfacial contact of heterojunction photocatalysts has a significant contribution in separation of interfacial charge carriers for photocatalytic hydrogen (H 2 ) evolution in a more efficient manner. Herein, an internal electric field (IEF)-induced S–scheme system comprised of two-dimensional (2D) CoAl layered double hydroxide (LDH) and 2D molybdenum disulfide (MoS 2 ) was constructed via a simple hydrothermal process. In the presence of visible-light irradiation, the 2D/2D MoS 2 /CoAl LDH hybrid demonstrates eightfold greater photocatalytic H 2 generation rate as compared with that of CoAl LDH. The mechanism was investigated in the light of the results of the X-ray photoelectron spectroscopy (XPS) and work-function calculated by density functional theory (DFT) simulation, and the improved activity was ascribed to that the rapid detachment of the electron-hole (e − -h + ) combinations and high redox ability, both are simultaneously realized in MoS 2 /CoAl LDH hybrid with a 2D/2D S–scheme charge transfer mechanism induced by the IEF across interface of the MoS 2 and CoAl LDH. Furthermore, favorable 2D/2D structure and better H* adsorption behavior of MoS 2 /CoAl LDH also promoted the improvement of water reduction performance. This work is a valuable guideline in developing of IEF-induced S–scheme photocatalysts with 2D/2D architecture for improved photocatalytic performance.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Dan Huang,Shuangshuang Tan,Maosheng Li,Dandan Wang,Chunhua Han,Qinyou An,Liqiang Mai
The application of high-energy Mg/S batteries was obstructed by the insufficiency of low-cost and non-nucleophilic electrolyte. In this work, a non-nucleophilic electrolyte was prepared by facilely dissolving Mg(CF3SO3)2, MgCl2, and AlCl3 in 1,2-dimethoxyethane (DME). The equilibrium species of the MTB electrolyte mainly comprise [Mg2(μ-Cl)2(DME)4]2+ and [(CF3SO3)AlCl3]−, which are generated by dehalodimerization reaction and Lewis acid–base reaction, respectively. The electrolyte exhibits a highly efficient reversible Mg deposition/dissolution, low overpotential of around 250 mV, and good oxidative stability up to 3.5 V after conditioning. The conditioning process that the active [Mg2(μ-Cl)2(DME)4]2+ species transforms into [Mg3(μ3-Cl)(μ2-Cl)2(DME)7]3+ was demonstrated, owing to the irreversible deposition of Al3+ on Mg foil. More importantly, this electrolyte exhibited good compatibility and kinetics for reversible Mg/MgSx redox, resulting in a high specific capacity of 866 mAh g–1 at 200 mA g–1 and high power density of 550 W kg–1. This work offers a new direction for low-cost, non-nucleophilic electrolyte and paves the way to explore high-power Mg/S batteries.
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Nanoscale
·
2020
·Vol. 12
·期 27
·14863-14869
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IF 6.895
Shuli Yin,You Xu,Songliang Liu,Hongjie Yu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
The development of doped noble metal catalysts with nonmetal elements to improve the catalytic performance toward the oxygen reduction reaction (ORR) is significant for proton exchange membrane fuel cell technology. Here, we report a one-pot for dual-nonmetal-doping strategy for the synthesis of S and P-co-doped mesoporous PtPd nanocages (PtPdSP mNCs) by using pre-synthesized mesoporous PtPd nanocages (PtPd mNCs) as the precursor and triphenylphosphine sulphide as both S and P sources. Benefitting from the combined advantages of metal–nonmetal incorporation, hollow cavity and surface porosity, the resultant quaternary PtPdSP mNCs exhibit outstanding ORR activity and long-term stability. This research work provides a good strategy for the doping of two or more selected nonmetallic elements into metallic nanocrystals with a controllable structure and composition.
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Nano Energy
·
2020
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IF 16.602
Qing Yu,Jiangjian Shi,Linbao Guo,Biwen Duan,Yanhong Luo,Huijue Wu,Dongmei Li,Qingbo Meng
For Cu 2 ZnSn(S,Se) 4 (CZTSSe) solar cells, eliminating multi-layer crystallization is a key issue of achieving high quality CZTSSe absorber layers and high cell performance. In this work, the formation mechanism of the multi-layer crystallization is revealed, that is, the reaction between CZTS and Mo may give the secondary phase, which subsequently acts as crystal nucleus to facilitate the CZTSSe crystal growth at back interface (Mo/CZTSSe), leading to multi-layer crystallization. By introducing MoO 3 isolating layer, this undesired reaction can be well prevented, and high quality single-layer crystals are obtained. This absorber film with fewer defects and secondary phases exhibits better semiconductor properties . Based on this regulated CZTSSe absorber layer, 11.68% (active area: 0.16092 cm 2 ) and 10.69% (mask area: 0.17586 cm 2 ) certified power-conversion-efficiency have been achieved with significant increase in the open-circuit voltage and fill factor.
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Biomass Conversion and Biorefinery
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2020
·Vol. 12
·期 9
·3933-3942
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IF 2.602
Xu Lu,Wang Aili,Li Siqiang,Zhang Liya,Pan Ruiyu,Guo Peng,Yi Ming,Liu Jie
Biomass residue cellulose-based poly-(ionic liquid)s (ILs) were in situ synthesized via activators generated by electron transfer for atom transfer radical polymerization in ionic liquid microemulsions. These biomass residues, including apple residue, citrus residue, and ginkgo leaf, were started with pretreatment and modification in ionic liquid microemulsions, and their structure and thermal stability were significantly altered before and after modification as confirmed by scanning electron microscopy and thermogravimetric analysis. Fourier-transform infrared spectroscopy and 31 P nuclear magnetic resonance spectroscopy were used to investigate the molecular structure of the biomass residue cellulose-based poly-ILs. In addition, the adsorption performance of the biomass residue cellulose-based poly-IL adsorbents for heavy metal ions, such as Cd(II), Zn(II), Cr(IV), Cu(II), Mn(II), Ni(II), and Pb(II), in water were investigated. Results show that the prepared adsorbent possesses good thermal stability and certain adsorption capacity for metal ions in water, especially for nickel ions (93.91 mg/g). The prepared adsorbent also exhibits remarkable performance in the field of biomass residue utilization and novel poly-IL adsorbents.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2019
·Vol. 137
·期 26
·48830
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IF 2.188
Gang Wang,Fei Wang,Anfeng Li,Miaomiao Zhang,Jie Zhang,Jinwei Chen,Ruilin Wang
The SPEEK/s-TiO 2 composite membrane was prepared by blending sulfonated poly(ether ether ketone) (SPEEK) and sulfonated titanium dioxide (s-TiO 2 ) nanoparticles. The important physiochemical parameters such as proton conductivity, water uptake, swelling degree and ion exchange capacity of the composite membrane were measured. The thermal stability and chemical stability were also tested. It was observed that the SPEEK/s-TiO 2 composite membrane exhibited the best selectivity (7.13 × 10 4 S·min·cm −3 ) accompanying high proton conductivity (0.061 S·cm −1 ) and low tetravalent vanadium ion (VO 2+ ) permeability (8.55 × 10 −7 cm 2 ·min −1 ) compared with Nafion117, SPEEK and SPEEK/TiO 2 membranes. The battery performance with these membranes was characterized by charge–discharge cycling tests and it was found that the SPEEK/s-TiO 2 composite membrane showed the highest energy efficiency (EE) up to 82.3%, indicating the SPEEK/s-TiO 2 composite membrane is a candidate for vanadium redox flow battery (VRFB) application. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2020 , 137 , 48830.
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MACROMOLECULAR RESEARCH
·
2019
·Vol. 28
·期 5
·450-454
·
IF 1.758
Gu Yiyang,Zhao Zhen,Chao Danming,Liu Xincai
Stimuli-response materials have attracted considerable attention due to their potential applications in sensoring, smart coatings, and intelligent devices. Herein a novel thermo-photo staged response shape memory poly(aryl ether ketone) bearing flexible alkyl segments and azobenzene groups was successfully designed and synthesized. Its chemical structure, thermostability and mechanical properties were characterized through Fourier Transform infrared spectroscopy, nuclear magnetic resonance spectroscopy, thermal gravimetric analysis and dynamic mechanical analysis. The resultant polymer disclosed thermo-/photo-dual stimuli-response behaviors, ascribed to its unique chemical structure. Firstly, the polymer film exhibited good thermal response shape memory effect with satisfied shape fixity ratio ( R f ) and shape recovery ratio ( R r ) (>99%). Moreover, an interesting photo-thermo two-staged responsive shape memory behavior with bending deformation over 100° upon the exposure of ultraviolet light and recovering to its original state through thermal treatment was revealed, attributed to the transcis isomerization of azobenzene groups.
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Journal of Materials Chemistry C
·
2022
·Vol. 10
·期 48
·18164-18173
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IF 8.067
Weifeng Kong,Zipeng Xing,Hang Zhang,Bin Fang,Yongqian Cui,Zhenzi Li,Peng Chen,Wei Zhou
A hollow polyhedral structure can effectively capture light and facilitate carrier separation, thus enhancing photocatalytic performance. Herein, hollow cubic CdS@CoS/WS2 dual S-scheme heterojunction superstructure photocatalysts are fabricated using a simple sulfidation and hydrothermal method. CdS@CoS/WS2 with a band gap of 1.59 eV and a relatively narrow band gap broadens the photoreaction to the near-infrared region and shows a good photothermal effect, which can promote photocatalytic reactions. It shows a relative specific surface area of 91.58 m2 g−1, which provides abundant surface-active sites to enhance the photocatalytic reaction. Under light conditions, the photocatalytic degradation ratios of CdS@CoS/WS2 for tetracycline and bisphenol A are up to 98.9 and 99.1%, and the hydrogen evolution efficiency is also up to 10.62 mmol h−1 g−1. The enhanced photothermal–photocatalytic performance could be due to the formation of a dual S-scheme heterojunction superstructure that facilitates space charge separation, a narrow band gap and a mesoporous hollow structure promoting solar light utilization, providing abundant surface-active sites and enhanced mass transfer. This simple strategy provides a new idea for the construction of high-performance hollow superstructure photocatalysts.
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ULTRASONICS SONOCHEMISTRY
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2022
·
IF 9.336
Jiabei Wang,Zhiqiang Jiang
A series of porous S-doped carbon nitride ribbons (PSCN) were prepared by one-pot hydrothermal and sonochemical synthesis techniques. The morphologies and nanostructures of the catalysts were characterized by SEM, XRD and IR, which confirmed the pristine graphitic structures of carbon nitrides retained in the products. Due to sonication treatment, PSCN has porous structures in the thin ribbon and larger specific surface areas (PSCN 43.5 m 2 /g, SCN 26.6 m 2 /g and GCN 6.5 m 2 /g). XPS and elemental mappings verified that sulfur atoms were successfully introduced into the carbon nitride framework. Diffuse reflectance spectroscopy (DRS) results showed S-doping in the carbon nitride reduced the bandgap energy and enhanced their capability of the utilization of visible light, which contributed to higher photo-generated current. Photoluminescence (PL) analysis indicates the recombination of photogenerated carriers was suppressed in PSCN. Moreover, the photocatalytic performance showed that S-doping and porous and thin ribbon nanostructures may effectively boost the CO 2 reduction rate (to as much as 5.8 times of GCN) when illuminated by visible light (>420 nm) without the need of sacrificial materials. The preliminary mechanisms of the formation of PSCN and its applications in photocatalytic CO 2 reduction are proposed. It highlights the potential of the current technique to produce effective, nonmetal-doped carbon nitride photocatalysts.
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SOLID STATE SCIENCES
·
2023
·
IF 3.5
Dong Gao,Fuqiang Chen,Hongping Wu,Zhanggui Hu,Jiyang Wang,Yicheng Wu,Hongwei Yu,P Shiv Halasyamani
Heteroanionic materials are of current research interest owing to their varied structural chemistry and properties. Recently, a number of heteroanionic materials have been synthesized that can be used for water splitting, battery materials, thermoelectrics , and nonlinear optical applications. Birefringent heteroanionic materials are still rarely researched. Herein, we report a series of new oxychalcogenides, AGe 2 O 4 Q (A = Ba, Sr; Q = S, Se), that are synthesized by solid-state reactions in fused silica tubes with their structures determined by single-crystal X-ray diffraction. Optical property measurements show that AGe 2 O 4 Q (A = Ba, Sr; Q = S, Se) exhibit large birefringences , 0.13–0.19 @ 1064 nm. These are one-order of magnitude larger than their single-anionic homologue, BaGe 2 O 5 - 0.03 @ 1064 nm. This suggests that constructing heteroanions through using chalcogenides to partially substitute O in tetrahedral foundation building units (FBUs) is a viable method for designing new birefringent materials. Furthermore, the crystal structures, UV–vis–NIR diffuse reflectance spectra, infrared and Raman spectra as well as the first-principles calculations for AGe 2 O 4 Q (A = Ba, Sr; Q = S, Se) are also reported.
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