ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Yong Zeng,Yizhen Chen,Di Sha,Yuchao Wu,Renhui Qiu,Wendi Liu
Thermoplastic polyurethane (TPU) elastomers are widely used in daily products owing to their flexible structures and decent mechanical properties. Vegetable oils (VOs) are promising renewable resources for polymer synthesis with readily availability and abundant derivatives. However, most VO-based polyurethanes are usually thermosets with an unsatisfactory material performance because the C═C bonds are randomly located on triglyceride long chains. Herein, a biobased TPU elastomer was facilely synthesized from palm oil (PO) with desirable and tunable mechanical properties. PO-based diol was synthesized from PO via amidation with 2-(2-hydroxyethylamino)ethanol. The resulting PO diethanolamide (POEA), combined with biobased butane-1,4-diol, was further reacted with 1,6-diisocyanatohexane to prepare PO-based TPU elastomers. The elastomers containing abundant H-bonds from carbamates in the backbone and dangling fatty acid side chains exhibited a microphase separation structure, endowing the elastomers with superior stretchability (up to a strain of 831%), restorability, and self-healing ability. The morphological, melting, crystallization, and rheological behaviors of the elastomers were fully studied. The dynamic and reversible three-dimensional cross-linked network consisting of van der Waals forces and H-bonds was investigated to reveal the formation mechanism of the elastomers.
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ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Xiang Meng,Jianlong Wang,Lejin Xu
To further improve the treatment capacity of actual wastes, H + was introduced into the homogeneous Fenton system as a co-catalyst for dissolution and degradation of the mixed nuclear-grade cationic and anionic exchange resins. The effects of acid type and concentration, catalyst type and concentration, H 2 O 2 dosage, initial temperature, antifoaming agent and resin ratio were studied. The concentration of inorganic acid , type and concentration of catalyst had significant influence on the decomposition of mixed resins. The experimental results showed that when the mixing ratio of resins was 1:1, the initial temperature was 96 ± 1 °C, the amount of H 2 O 2 was 200 mL, and the concentration of H + /Fe 2+ was 1 M/0.1 M, complete dissolution and 79% weight reduction of mixed resins were obtained. Combined with density functional theory (DFT) calculations, cationic exchange resin and anionic exchange resin showed different reactivity in the experiment. Hydroxyl radicals (•OH) tended to attack –SO 3 - groups with more negative charges, and the barrier energy of –SO 3 - ion dissociation was 8.2 kcal/mol, which caused the cationic exchange resin to be easily destroyed. According to the characterization results, the characteristic intermediates were determined, indicating that desulfonation, valence change of nitrogen atom , and cleavage of long-chain carbon skeleton existed during the reaction, but incomplete oxidation still remained.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Dongxue Zhou,Xiangdong Xue,Xing Wang,Qingjie Luan,Ang Li,Liguo Zhang,Baozhen Li,Wenjun Dong,Ge Wang,Changmin Hou
Element doping is an excellent strategy to promote charge separation and reaction kinetics of photocatalyst, which plays significant role in accelerating the sustainable energy development process. Herein, Ni, In co-doped ZnIn 2 S 4 photocatalyst was prepared by a microwave-assisted solvothermal method. The rapid crystallization of ZnIn 2 S 4 resulted in partial In atoms substituted Zn atom during the formation of [ZnS] 4 layer. In doping in tetrahedral Zn sites increases the electron delocalization around In sites, hence reduces the electronic potential wells along Z axis. Ni doping in tetrahedral Zn sites decreases the negative charge on the S sits, which balances the H adsorption/desorption, further boosting the photocatalytic activity. As a result, Ni, In co-doped ZnIn 2 S 4 possess an optimal photocatalytic H 2 evolution property of 21.94 μmol·h −1 , which is nearly 1.8 and 6.1 times of In-ZnIn 2 S 4 (11.78 μmol·h −1 ) and ZnIn 2 S 4 (3.6 μmol·h −1 ).
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Heng Ye,Shengnan Wang,Yong Wang,Peiting Guo,Liying Wang,Chengke Zhao,Shuqing Chen,Yimai Chen,Hongqi Sun,Shaobin Wang,Xing Ma
Wastewater remediation using micro/nanomotors is a hot topic, and MnO 2 based materials have become fascinating alternatives to rare noble metal-based micro/nanomotors. Herein, we demonstrate facile and large-scale synthesis of Fe-MnO 2 core-shell micromotors for antibiotic pollutant removal. Heat-treatment results in a phase transformation of MnO 2 with formation of iron oxides and partially exfoliates the MnO 2 nanoplate shell structure to promote mobility. The iron-manganese oxide micromotors exhibit an efficient removal of tetracycline antibiotics via a combination of catalytic degradation and adsorptive bubble separation. For the first time, atomic H* was found to participate in the micromotor-assisted degradation process, resulting in optimal Fenton reaction in neutral conditions with a good decontamination performance. Owing to the merits of abundance, magnetic recovery, facile fabrication, good motion, and environmental friendliness, as well as decontamination performance in a wide pH range, these core-shell micromotors demonstrate a promising candidate in practical wastewater treatment .
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Catalysis Science & Technology
·
2022
·Vol. 12
·期 6
·1788-1798
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IF 6.177
Jing Zhao,Yanzhuo Zhang,Hucheng Zhang,Haiyan Wang,Jianji Wang
Hydrogen spillover is an important theme for hydrogen storage and H-involving catalytic reactions. This work shows that catalytic reactivity and selectivity can be revealed by differentiating the energetic characteristics of spilled H species. With the assistance of Ti, F and C in MXenes, Pd1.8Ni@Ti3C2Tx presents a high capacity for spillover hydrogen storage at ambient temperatures, and the rich oxygenated groups act as the main carriers of hydrogen spillover around metal nanoparticles. Thermodynamic analysis reveals that the catalytic performances are energetically dominated by the adsorption enthalpies of the active spilled H species rather than the amount of spillover hydrogen, and can be tuned by alloying and surface modification. The ideas are verified from the excellent catalysis, chemoselectivity and stereoselectivity of Pd1.8Ni@Ti3C2Tx in semihydrogenations. The strategy of maximizing catalytic performances is applicable to other Pd-based bimetals@Ti3C2Tx, such as Pd2.6Co@Ti3C2Tx and Pd1.5Fe@Ti3C2Tx, and provides new energetics perspectives to understand the catalytic mechanism in spillover-involving chemical procedures.
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JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 141
·期 6
·e54911
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IF 3
Mengqing Ren,Zixin Wu,Lili Wu,Bing Yu,Weilin Wu,Baoying Liu,Shengqiang Xiao
The pulley structure has been widely employed to improve mechanical properties. Polyrotaxane-based waterborne polyurethane (WPU) typically exhibits good tensile strength and Young's modulus. However, achieving outstanding self-healability of polyrotaxane-based WPU under mild conditions generally proves insufficient solely relying on host-guest interactions. Herein, a strategy that constructs a triple synergy of host-guest interaction, hydrogen bonds, and metal coordination bonds by sequentially introducing tannic acid (TA) and Fe 3+ is proposed to prepare polyrotaxane-based WPU with excellent mechanical performance and high self-healable capability. Besides the reversible non-covalent bonding contributing to intrinsic self-healing, the unique sliding motion of WPU's molecule chain acts as a driving force, promoting efficient contact among reversible bonds. Notably, benefiting from the sliding motion of β-cyclodextrin (β-CD) along a chain, the dynamic reconstruction of hydrogen bonds and metal coordination bonds, the resulting supramolecular WPU exhibited a tensile strength of 46.05 MPa and a toughness of 130.30 MPa, with satisfactory self-healing performance (tensile strength healing efficiency of more than 95%). This work enriches the self-healing mechanism and expands the concepts for the design of resilient self-healing environmentally friendly supramolecular WPU.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Ruokun Jia,Jiayuan Deng,Xiaohang Yang,Ruisong Xue,Pengpeng Wang,Xingbo Bian,Qiyao Wang
Graphitic carbon nitride (CN) hold great promise as a photocatalyst for generating hydrogen energy via water splitting, owing to its remarkable ability to respond to visible light and its strong reduction capacity. However, the photocatalytic water splitting for H 2 evolution performance of pure CN was impeded by its low surface area, inadequate hydrophilicity, and unsatisfactory photoelectric conversion efficiency. Here we tackled these challenges by synthesizing a series of CN/H-ZSM-5 composites with varying amount of H-ZSM-5 zeolite using a straightforward thermal copolymerization method. The contact angle and N 2 adsorption-desorption measurements confirmed that the incorporated hydrophilic and porous H-ZSM-5 zeolite contribute to increased surface area and improved hydrophilicity of the CN/H-ZSM-5 composites. Meanwhile the resulting CN/H-ZSM-5 composites exhibited significant separation and migration enhancement of photoexcited charge carriers. Consequently, the optimized CN/H-ZSM-5 composite, containing 50 mg of H-ZSM-5 zeolite, demonstrated 13 times increase in photocatalytic H 2 production rate than that of pure CN. This work not only provided a competitively universal approach on the design of high-efficiency CN based photocatalyst, but also clarified the role of H-ZSM-5 zeolite in the H 2 evolution enhancement.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 40
·18865-18871
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IF 3.3
Chao Liu,Gang-Gang Chang,Ting-Ting Luo,Yi-Tian Wang,Shi-Tian Xiao,Yao Yao,Hong-Jian Xu,Ge Tian,Christoph Janiak,Hai-Hu Yu,Xiao-Yu Yang
Metal–organic frameworks (MOFs) have great potential for producing photoelectrocatalyzed hydrogen and degrading pollutants, owing to several factors such as high porosity and tunable semiconductor-like properties. Wide band gaps, which restrict their use to only UV light induced reactions, and low efficiencies for the separation of photogenerated charge carriers (electrons and holes) pose significant challenges to the widespread applications of MOFs. In this study, a hierarchical hollow Pt@H-UiO-66-NH2/CdS ternary catalyst was designed and synthesized. The immobilized CdS nanoparticles (NPs) in this catalyst endow the MOF H-UiO-66-NH2 with high visible light absorption ability and the Pt NPs serve as electron sinks to improve charge carrier separation. Furthermore, the hierarchical hollow structure of H-UiO-66-NH2 in the composite contributes to boosting light absorption and shortening the distance for charge transfer. As a proof of principle, Pt@H-UiO-66-NH2/CdS catalyzes methylene blue (MB) degradation with a high rate constant of 1.025 × 10−2 and hydrogen production with a rate of 12 810 μmol g−1 h−1, the latter of which is about 2.3, 11.7 and 173 times higher than those of Pt@UiO-66-NH2/CdS, H-UiO-66-NH2/CdS and Pt@H-UiO-66-NH2, respectively.
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2021
·Vol. 306
·期 8
·2100159
·
IF 4.367
Hanglan Qin,Yajun Chen,Jieyu Huang,Qufu Wei
Hydrogel, as a promising soft material, possesses many functional advantages such as stretchability, viscoelasticity, and biocompatibility. An advanced electronic platform for strain sensor is constructed by modifying hydrogels with various doping techniques. Herein, a novel flexible conductive hydrogel is synthesized by combination of bacterial cellulose/sodium alginate/polyacrylamide with the polyaniline (BSP-PANI) through multiple intermolecular interactions. In the obtained BSP-PANI hydrogel system, the incorporated BC serves the function of mechanically toughening and the formation of polyaniline conducting network endows the hydrogels electrical conductivity. The assembled hydrogel strain sensor can detect electrical response under different applied strains (1–200%) and monitor human motion in real time. Therefore, it is believed that the BSP-PANI hydrogel prepared by the feasible synergetic strategy proposed in this work has greatly diversified application in smart epidermal sensors and artificial intelligence devices.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2020
·
IF 3.232
Chenxiao Yan,Qingqing Zhang,Heng Gao,Xiong Zheng,Tong Yang,Guoxiang Zheng,Xiaoshun Zhou,Yong Shao
DNA templated dye assemblies pave an easy way to regulate the optical properties of molecular aggregates. G-quadruplexes (G4s) provide versatile DNA platforms for the dye assemblies since their foldings can be easily tuned by cation ions and sequences. In this work, we found that the G4 handedness can be used to control the aggregate chirality of a dye of 3,3′-diethylthiacarbocyanine (DiSC 2 (3)). The left-handed and right-handed G4s can template the concurrent formation of the J- and H-aggregates of DiSC 2 (3) with emergence of the featured absorption spectra. However, the chiral J-aggregate of DiSC 2 (3) can be formed only on the left-handed G4s, while the chiral H-aggregate is otherwise grown only on the right-handed G4s, as confirmed by the induced circular dichroism (ICD) spectra with the characteristic splitting bands. Additionally, these G4s even at tens of nM level are efficient to produce these chiral aggregates, demonstrating the high sensitivity of G4s in creating these optically active dye assemblies. The possible growth sites of the aggregates are proposed by the sequence length-dependent assemblies. Our work will provide a new way to control the chiral assemblies of dye aggregates via the G4 handedness.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 35
·16455-16469
·
IF 3.553
Zhang Zengqi,Wang Qiang,Zhang Mingzhong,Huang Zongxian,Zhuang Shiyu
The filler effect is the most important physical mechanism of mineral admixtures in the early hydration of cement whose chemical properties greatly affect the precipitation of C–S–H. In this study, calcite, strontianite, magnesite, dolomite, quartz, whewellite and whitlockite were selected as the fillers. The morphology and reaction kinetics of synthetic C–S–H precipitated on the surfaces of different fillers were studied via electron microscopy observations and electrical conductivity and ion concentration measurements. The precipitation rate of C–S–H has a positive correlation with the affinity of Ca 2+ for adsorption on the fillers, which can be explained by the nucleation barrier of C–S–H. Extremely ordered honeycomb-like morphology of the C–S–H is found on calcite and strontianite surfaces, while less regular leaf-like or honeycomb-like C–S–H is found on whewellite and whitlockite. The ordered C–S–H pattern is related to the lattice cleavage of the ionic compound filler. In the case of quartz, C–S–H prefers growth along the tangential direction, which is quite different from the normal-direction growth on ionic compounds. The in-plane growth of C–S–H on quartz is believed to be induced by a layer of loosely physically adsorbed Ca 2+ .
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ACS Omega
·
2020
·
IF 2.87
Ning Song,Shao-Peng Chen,Xiao-Wei Fan,Yu-Hui Tan,Wen-Juan Wei,Yun-Zhi Tang
The molecular design and regulation has shown bright future for constructing smart molecular materials such as ferroelectrics, dielectric switches, electro-optic effect, and so forth. Here, by poly-H/F substitution in a simple organic-inorganic hybrid 2[CH2FCH2NH3]·[CdCl4], 1 (CH2FCH2NH3 = fluorine ethylamine cation), we obtained two novel hybrids, namely, 2[CHF2CH2NH3]·[CdCl4], 2 (CHF2CH2NH3 = 2,2′-difluorine ethylamine cation) and 2[CF3CH2NH3]·[CdCl4], 3 (CF3CH2NH3 = 2,2′,2″-trifluorine ethylamine cation). Further investigations show that compounds 1, 2, and 3 experience solid reversible phase transitions with temperatures at 294, 319, and 329 K respectively. These unique phase transitions were confirmed by their remarkable dielectric and heat anomalies around the phase transition temperatures. X-ray single-crystal diffraction analyses before and after the phase transitions show that the order–disorder motions of F atoms and the twist motions from the 2D [CdCl4]2– framework lead to these solid reversible phase transitions. Also, the Hirshfeld surface calculation of compounds 1, 2, and 3 suggests that the increasing ratio of the F···F interaction from the intermolecular interaction makes a major contribution for the substantial increase of their phase transition temperatures.
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