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JOURNAL OF MATERIALS SCIENCE · 2022 ·Vol. 57 ·期 27 ·12836-12847 · IF 4.682

Copper containing 3D polyaniline/phytic acid hydrogels for photocatalytic hydrogen production

Pan Xueling,Wu Sheng,Wang Tingting,Histand Gary,Li Yingwei

Abstract A Cu-PP hydrogel with 3D network was synthesized using a simple in-situ polymerization method. PA (phytic acid) acts as the dopants and crosslinking agent to form PANI-PA (polyaniline-phytic acid) hydrogel via in-situ polymerization of aniline. PA is also used as a chelating agent to coordinate with Cu 2+ ion due to the high coordination capacity. When irradiated by light, Cu 2+ was slowly reduced to form Cu NPs, distributing uniformly in the 3D matrix of PANI-PA. The 3D network nanostructure ensures a complete contact between the photocatalyst and water, promoting the separation of electrons and holes. The introduction of PANI-PA improves the separation efficiency of electron-hole pairs, where PANI-PA acts as a hole reservoir to trap the holes generated by Cu NPs, hindering the recombination of electron-hole pairs. The Cu 0.2 -PP hydrogel with a copper content of 30.8% exhibits the best hydrogen production rate (6.09 mmol·g −1 ·h −1 ), which is 6.7 times greater than that of pure Cu NPs. Graphical abstract

研究领域: 材料科学 · 能源科学
✓ 已验证 DOI 高影响因子
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2019 · IF 14.229

Carbon dots-Pt modified polyaniline nanosheet grown on carbon cloth as stable and high-efficient electrocatalyst for hydrogen evolution in pH-universal electrolyte

Qian Dang,Yuyang Sun,Xiao Wang,Wenxiang Zhu,Ying Chen,Fan Liao,Hui Huang,Mingwang Shao

Design and fabrication of hydrogen evolution reaction (HER) electrocatalysts with high activity, durability and moderate price are vital for realizing a viable water-splitting technology. Here, we demonstrate the carbon dots-Pt modified polyaniline nanosheets grown on carbon cloth (CDs/Pt-PANI) can serve as stable and high-efficient electrocatalyst in pH-universal electrolyte for HER. The overpotential for optimal CDs/Pt-PANI electrocatalyst can be lowered to 30 mV at 10 mA·cm −2 when Pt loading was only 8.1 μg·cm −2 (the Pt content in commercial 20 wt% Pt/C is 22.4 μg·cm −2 ), showing exceptional HER efficiency with a small Tafel slope 41.7 mV·dec −1 in acidic solution. Meanwhile, the optimal CDs/Pt-PANI electrocatalyst exhibits well stability with 17 mV potential shift after 20 h, which is 0.06 times than that of commercial 20 wt% Pt/C (286 mV). It is noticeable, the optimal CDs/Pt-PANI electrocatalyst is superior to 20 wt% Pt/C with HER performance in pH-universal electrolyte (acidic, neutral and basic). The efficient and stable HER performance of CDs/Pt-PANI should ascribe to the synergy in the CDs, Pt and PANI, in which the surface functional groups of CDs can connect tightly with PANI and improve the stability of Pt, simultaneously, the PANI and Pt provide the high-efficiency in HER.

研究领域: 材料科学 · 电化学
✓ 已验证 DOI 高影响因子
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KEY ENGINEERING MATERIALS · 2019 · IF 0

Study on Catalytic Steam Reforming of Toluene over Ni/Activated Carbon Catalysts Prepared from Adsorption Treatment of Nickel Electroplating Wastewater by Activated Carbon

Xiao Fang Chen,Ning Jiang,Song Hu,Li Mo He,Guang Liao,Qiang Qiang Ren,Sheng Su,Yi Wang,Jun Xiang,Ji Hua Qiu

The conditions (adsorption duration and pH) for removal of nickel ions from nickel electroplating wastewater by adsorbing on activated carbon were studied. Ni/AC catalysts prepared by adsorption under alkaline conditions with high removal rate of Ni(II) has been chosen for catalytic steam reforming of toluene, and its catalytic performances were evaluated compared to that of Ni/AC catalysts prepared by impregnation. Alkaline conditions facilitated the removal of Ni(II) from nickel electroplating wastewater by AC and pH=9 in especial, was a critical point above which Ni(II) could be removed efficiently. The removal rate within 20 min reached up to more than 97%. After H2 reduction, the catalytic activity of Ni/AC-Ad was observed in catalytic steam reforming of toluene and then gradually decreased with the reaction time. Both the toluene conversion and hydrogen production with Ni/AC-Ad were about 65% of those with Ni/AC-Im at similar Ni loading rate. Under alkaline conditions, most of the nickel adsorbed on AC was Ni(OH)2 complex. This adsorption state led to a larger average size of nickel particle in Ni/AC-Ad than that in Ni/AC-Im. The uneven size of nickel particles on the surface caused poor dispersion of active spots, agglomeration and sintering, resulting in gradual deactivation of Ni/AC-Ad prepared under alkaline conditions during catalytic steam reforming of toluene.

研究领域: 环境科学 · 催化化学
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Chemistry-An Asian Journal · 2020 ·Vol. 16 ·期 2 ·165-173 · IF 4.056

Preparation of PdAuCu/C as a Highly Active Catalyst for the Reduction of 4-Nitrophenol by Controlling the Deposition of Noble Metals

Ying Duan,Yangyang Ma,Yanfu Xie,Dongmi Li,Dongsheng Deng,Chi Zhang,Yanliang Yang

The reasonable control of the dispersion of noble metals is an important topic for heterogeneous catalysts. In this manuscript, PdCu/C, AuCu/C and PdAuCu/C were prepared by the galvanic reduction method to ensure that Pd and Au follow the distribution of Cu nanoparticles. The catalysts were characterized by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), energy-dispersive spectrometer elemental mappings and lines scans. Both the Pd and Au had very high dispersion no matter whether they were introduced individually or simultaneously. The Pd and Au were distributed mainly on the Cu nanoparticles as evidenced by the energy-dispersive spectrometer elemental mappings and lines scans. The reduction of 4-nitrophenol was used as a model reaction for the prepared catalysts. PdCu/C and AuCu/C showed high activity for this reaction compared to the literature, and the activity could be further increased by the introduction of Pd and Au in an appropriate ratio at the same time. The normalized reaction rate reached 2.005 s −1 mM −1 for the PdAuCu/C-2.0, in which the mole ratio of Pd to Au was 2.0.

研究领域: 材料科学 · 催化化学
✓ 已验证 DOI 高影响因子
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JOURNAL OF ENVIRONMENTAL MANAGEMENT · 2022 · IF 8.91

Effect of rhamnolipids on the biodegradation of m-dichlorobenzene in biotrickling filters: Performance and mechanism

Bairen Yang,Jiajie Wang,Menglei Wu,Qingqing Shang,Hao Zhang

In this study, the effect of rhamnolipids (RL) on m -dichlorobenzene ( m -DCB) removal and biofilm was investigated in two biotrickling filters (BTF) (BTF1: blank control; BTF2: RL addition). The critical micelle concentration (CMC) value of RL was 75.6 mg L −1 , and the RL could significantly improve the solubilization of m -DCB. The results showed that the optimal concentration of RL was 180 mg L −1 . The removal efficiency (RE) of m -DCB dropped by 42.4% for BTF1 no fed with RL and only 28.2% for BTF2 fed with RL when the inlet concentration increased from 200 to 1400 mg m −3 at an empty bed time (EBRT) of 60 s. RL increased the secretion of extracellular polymers (EPS) and the ratio of Protein/Polysaccharide, which improved the mass transfer of m -DCB to the biofilm. RL also had a facilitating effect on catechol-1,2-dioxygenase (C 12 O) enzyme activity . Furthermore, RL increased Zeta potential and facilitated microorganisms to form biofilm . The dominant microorganisms of microbial community were increased and the application of RL promoted the enrichment of them.

研究领域: 环境工程 · 微生物学 · 生物技术
✓ 已验证 DOI PubMed 高影响因子
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Catalysis Science & Technology · 2020 ·Vol. 10 ·期 5 ·1467-1476 · IF 5.721

Enhancing the matching of acid/metal balance by engineering an extra Si–Al framework outside the Pd/HBeta catalyst towards benzene hydroalkylation

Zhuo-Qian Li,Xinxin Fu,Caiyan Gao,Jinyu Huang,Baojun Li,Yongpeng Yang,Jie Gao,Yonglong Shen,Zhikun Peng,Jing-He Yang,Zhongyi Liu

The one-step hydroalkylation of benzene to cyclohexylbenzene (CHB) needs to occur on bifunctional metal/zeolite catalysts, and introducing more acid sites to match the metal sites plays a key role in improving the matching of acid/metal sites toward the requirements of benzene hydroalkylation. Herein, we designed and constructed a Si–Al framework coating with extra acid sites outside the surface of the Pd/HBeta catalyst and obtained a zeolite-encaged Pd NP structure (Pd@HBeta). Notably, the Pd@HBeta catalysts achieved excellent catalytic performance with 44.0% CHB selectivity at about 85.0% benzene conversion, which is much higher than that of the Pd/HBeta catalyst with a CHB selectivity of 25.1% at the same benzene conversion. The remarkable increment of CHB selectivity of Pd@HBeta is mainly attributed to the extra acid sites provided by the coated Si–Al framework as well as the increase of the B/L ratio. Moreover, the adsorption capacity of benzene and cyclohexene is greatly improved after introducing extra acid sites by coating the Si–Al framework, which is beneficial for both hydrogenation and alkylation. Further DFT calculations reveal that C6H10 can easily desorb from Pd NPs and migrate to the acidic channel of HBeta in the Pd@HBeta catalyst than that in Pd/HBeta. Our work presents an elegant example of catalytic hydroalkylation selectivity regulation by coating an extra Si–Al framework to enhance the matching of acid/metal balance.

研究领域: 催化 · 化学工程 · 材料科学 · 物理化学
✓ 已验证 DOI 高影响因子
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Science China-Technological Sciences · 2017 ·Vol. 60 ·期 5 ·749-757 · IF 1.719

Ternary Fe3O4@PANI@Au nanocomposites as a magnetic catalyst for degradation of organic dyes

Zhu YuMei,Zhou XiaoWei,Chen DongSheng,Li Fang,Xue Tao,Farag Ahmed Saad

Magnetic Fe 3 O 4 @PANI@Au nanocomposites are fabricated through electrostatic self-assembly and seed growth methods. The rate constant K app is calculated to be 8.63×10 −3 s −1 at room temperature for the reduction of 4-nitrophenol to 4-aminophenol with an excessive amount of NaBH4 as a model system showing outstanding catalytic efficiency and stability. For recyclable performance, the catalyst exhibits slight loss in catalytic performance on the conversion of 4-nitrophenol after running for more than 10 cycles. Besides, the smaller and simpler the structure, the easier the molecular structure can be degraded, and the faster the cationic dyes can be degraded than the anionic dyes, which can reveal the selectivity. For practical application, Congo red as a pollutant of the lake water is degraded rapidly after Fe 3 O 4 @PANI@Au is added to the solution in a few minutes. It has been demonstrated that magnetic Fe 3 O 4 @PANI@Au nanoparticle composite is a promising catalyst for environment sewage.

研究领域: 纳米催化 · 环境化学 · 材料科学 · 污染治理 · 应用化学
✓ 已验证 DOI 高影响因子
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2022 · IF 4.326

Highly Interfacial Adhesion and Mechanism of Nylon-66/Rubber Composites by Designing Low-Toxic RF-like Dipping Systems

Shuangqi Diao,Wei Huang,Yingzhe Li,Wencai Wang,Bing Yu,Nanying Ning,Ming Tian,Liqun Zhang

Fiber-reinforced rubber composites (FRRC) are widely used as load-carrying and anti-pressure products. Resorcinol–formaldehyde–latex (RFL) dipping is widely used to improve interfacial adhesion between fiber and rubber in industry. Unfortunately, high volatility and toxicity of RFL do great harm to humans and the environment during the open dipping process. In this work, a phloroglucinol–terephthalaldehyde–latex (PTL) dipping system based on a low-toxic and low-volatile resin was developed to achieve equivalent interfacial adhesion instead of RFL ones. The reaction mechanism, chemical structure, and wettability changes on the Nylon-66 (PA66) fiber surface were characterized. The effect of the phloroglucinol/terephthalaldehyde (P/T) ratio on the dip pick-up, morphology of the fiber surface, and interfacial structure of FRRC was investigated to expound the interfacial adhesion mechanism. At the optimum P/T ratio (1/2.2), a dipping layer with uniform and suitable dip pick-up is achieved on the fiber surface, which ensures the formation of an appropriate graded interfacial layer with enough crosslinking density and modulus, under the synergistic effect of co-vulcanization with rubber, and accordingly strengthens interfacial adhesion. The dipped fiber possesses excellent interfacial adhesion, dynamic fatigue life, and storage stability at the RFL level. This new dipping system is environmentally friendly and easy to scale up without making any change in the process and equipment.

研究领域: 材料科学 · 高分子化学 · 环境工程
✓ 已验证 DOI 高影响因子
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Electrocatalytic oxidation of toluene into benzaldehyde based on molecular oxygen activation over oxygen vacancy of heteropoly acid

Ye Lv,Aiqun Kong,Houjun Zhang,Weiwei Yang,Yichong Chen,Menghui Liu,Yan Fu,Jinli Zhang,Wei Li

Benzaldehyde is much easier to be oxidized with respect to toluene, making the selective oxidation of toluene to benzaldehyde extremely challenging. Herein, a series of heteropoly acid catalysts with different ratios of molybdenum and vanadium supported on carbon paper (CP) were synthesized. The oxygen vacancy concentration and dispersion of heteropoly acid on CP can be changed by regulating the ratio of molybdenum and vanadium. Due to the suitable oxygen vacancy concentration and most uniform dispersion on CP, HPMoV 2 has the highest electrocatalytic oxidation performance, showing the benzaldehyde selectivity of 83.5% at the toluene conversion of 83.4%. In-situ Raman spectroscopy proved that toluene was initially activated into benzyl cation and further oxidized by active oxygen species (O 2 2- ads , O 2 - ads ) to form benzaldehyde. The active oxygen species generated by electro-activation of molecular oxygen adsorbed on oxygen vacancies of heteropoly acid, mainly contribute to the selective oxidization of toluene into benzaldehyde. This work develops a new electrochemical strategy to achieve highly selective conversion of toluene into benzaldehyde with molecular oxygen under mild conditions.

研究领域: 化学 · 催化 · 电化学 · 材料科学
✓ 已验证 DOI 高影响因子
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Molecular Catalysis · 2022 · IF 5.089

Molecular oxygen-promoted reconstruction of molybdenum phosphide enables selective electrochemical oxidation of p-chlorotoluene

Dongting Wu,Ye Lv,Wei Li,Yan Fu,Jinli Zhang

It is highly challenging to develop efficient catalysts for selective oxidation of p-chlorotoluene (PCT) into p-chlorobenzaldehyde (PCB) as PCB easily undergoes over-oxidation. Herein, a new electrochemical strategy was developed for selective oxidation of PCT with high selectivity toward PCB. A self-standing molybdenum phosphide (MoP) anode was directly synthesized on carbon cloth with the assistance of polyvinyl pyrrolidone. The as-synthesized MoP anode with 3D network structure, exhibits the selectivity of 91.4% toward PCB at the conversion of 75.6% in acetonitrile solution containing 0.1 M Bu 4 NClO 4 . During electrochemical oxidation, molecular oxygen-induced transformation of MoP into MoO 2 initiates the activation of PCT into ClC 6 H 5 CH 2 + . The ClC 6 H 5 CH 2 + reacts with molecular O 2 over electrode surface, producing the product of PCB. This work offers a promising strategy to achieve selective oxidation of C H bond based on electrochemical environment.

研究领域: 电化学 · 材料科学 · 催化 · 环境化学
✓ 已验证 DOI 高影响因子
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POLYMER BULLETIN · 2023 ·Vol. 81 ·期 6 ·5403-5420 · IF 3.2

A study of ortho-phthalimide functional benzoxazine resins with additional cross-linkable group

Liu Jiamei,Yang Rui,Sheng Weichen,Zhang Kan

Aromatic polyimides have attracted wide attentions in fields of aerospace, microelectronics and defense applications due to their outstanding thermal and mechanical performances. However, the rigidity originating from the imide structure attached with an aromatic ring causes difficulties in processing. In this study, we synthesized two ortho- phthalimide functional benzoxazine monomers with additional cross-linkable groups (including both furan and alkynyl). An ortho- phthalimide functional phenol, 2-(2-hydroxyphenyl) isoindole-1,3-dione ( o PP), was obtained by reacting o -aminophenol and phthalic anhydride in acetic acid. Two monofunctional ortho- phthalimide containing benzoxazine monomers ( o PP-fa and o PP-pa) were then synthesized using the Mannich reaction based on raw materials of o PP, furfurylamine/propargylamine and paraformaldehyde in toluene. The structures of benzoxazine monomers were confirmed by FT-IR and 1 H NMR spectroscopies. We also investigated effects of cross-linkable functionalities on curing behaviors as well as their corresponding polymerization mechanisms. The activation energies of o PP-fa and o PP-pa were calculated by Kissinger and Ozawa equations based on DCS measurements with different heating rates. It demonstrates that the exothermic peak temperature of o PP-pa is located at 178.5 °C, which is much lower than that of o PP-fa (223.3 °C). The alkyne group in o PP-pa plays a catalytic effect role in reducing the ring-opening polymerization temperature of the oxazine ring. Moreover, the thermogravimetric analyzer (TGA) was used to evaluate thermal properties of the obtained polybenzoxazine thermosets. Both thermosets exhibited improved thermal stability compared with some other reported monobenzoxazine-derived polybenzoxazines.

研究领域: 高分子科学 · 材料化学 · 热分析 · 有机合成
✓ 已验证 DOI 高影响因子
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Journal of Materials Chemistry B · 2020 ·Vol. 8 ·期 33 ·7428-7437 · IF 5.344

Bottlebrush-like highly efficient antibacterial coating constructed using α-helical peptide dendritic polymers on the poly(styrene-b-(ethylene-co-butylene)-b-styrene) surface

Yujia Zhang,Ke Kang,Nanhang Zhu,Guohao Li,Xiaoxi Zhou,Aimin Zhang,Qiangying Yi,Yao Wu

Infectious diseases induced by pathogenic bacteria are the major causes for the failure of medical implants. Meanwhile, the drug-resistance is steadily developed because of the large and even inappropriate use of antibiotics. Therefore, the development of antibacterial coating with non-antibiotic-based agents on the surfaces of medical implants and devices has been an urgent need. Herein, we propose a bottlebrush-like antibacterial coating on a poly(styrene-b-(ethylene-co-butylene)-b-styrene) (SEBS) triblock copolymer surface by UV-induced graft polymerization of poly(ethylene glycol) (PEG) acrylate terminated poly(lysine dendrimer). This PEG-conjugated antibacterial polymer possessed a substructure of α-helical backbone and cation dendrimer side chains stretching in the radial directions of the helix. The introduction of lysine peptide dendrimers endowed the prepared antibacterial polymer with precisely controlled characteristics of its local cation density, amphipathic composition as well as three-dimensional (3D) conformation to improve interactions with bacterial membranes. The antimicrobial assay and biocompatibility assay results showed that 96.83% of S. aureus and 99.99% of E. coli were killed after being in contact with the antibacterial coating, while no toxicity to mammalian cells or no hemolysis was detected. This antimicrobial activity was further confirmed by the molecular dynamics simulation results, which demonstrated that the employment of lysine peptide dendrimers enhanced the electrostatic interaction and hydrogen bonding between the brush and bacterial membranes remarkably. Such bottlebrush-like antibacterial coating constructed using α-helical peptide dendritic polymers may become an effective strategy for manufacturing antibacterial products for biomedical uses.

研究领域: 生物医学工程 · 材料科学 · 微生物学
✓ 已验证 DOI PubMed 高影响因子
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