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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Achieving high-efficient urea oxidation via regulating the rate-determining step over a V single atom incorporated Co hydroxide electrocatalyst

Baojie Zhang,Changti Pan,Hengjie Liu,Xingshun Wu,Hongliang Jiang,Li Yang,Zeming Qi,Guang Li,Lei Shan,Yunxiang Lin,Li Song,Yong Jiang

Urea oxidation reaction (UOR) has emerged as a competitive approach for many energy-related technologies due to the low overpotential and fast reaction dynamics. The main challenge lies in fabricating high-efficient catalysts with optimized electronic structure and understanding the intrinsic structure-related mechanisms. Here, we report a feasible strategy of regulating the rate-determining step (RDS) of UOR via an electrochemical reconstructed Co hydroxide catalyst incorporated with V single atoms. The optimal catalysts exhibit an enhanced UOR performance after V incorporation while remarkably suppressed the competitive oxygen evolution with the potential of 1.54 V (vs RHE) to achieve the current density of 30 mA cm −2 . Operando synchrotron-radiation Fourier transform infrared spectroscopy (SR-FTIR) combining density functional theory (DFT) calculations reveal that enabled by single atom V incorporation, the RDS of UOR has been changed from the first deprotonation step to the second one with a lower energy barrier of 2.05 eV (vs 2.6 eV), which is thermodynamically favorable for the overall reaction process.

研究领域: 电化学 · 材料科学 · 催化 · 能源技术
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GREEN CHEMISTRY · 2022 ·Vol. 25 ·期 2 ·596-605 · IF 11.034

Highly efficient and stable photocatalytic CO2 and H2O reduction into methanol at lower temperatures through an elaborate gas–liquid–solid interfacial system

Haitao Yu,Yimin Xuan,Qibin Zhu,Sheng Chang

It is extraordinarily exigent to solve the efficiency of 6H+/6e− photoreduction of CO2 and H2O into methanol as the major product, which is limited by the severe photogenerated carrier recombination, the reoxidation of methanol at high temperature, and photocorrosion of catalysts. Herein, we developed an elaborate gas–liquid–solid system assembled by using a novel multicomponent SrTiO3 (La Cr)/Cu@Ni/SiO2/TiN (STO/Cu@Ni/SiO2/TiN) heterojunction, realizing a highly efficient and robust photocatalytic CO2 reduction to methanol at low temperature. STO/Cu@Ni/SiO2/TiN exhibits excellent light absorption and high charge carriers separation nature, and the evolution of methanol is 25.8 μmol (h gcat.)−1 roughly not only 173 folds higher than those observed compared with the STO counterpart, but also is 50 times that those of traditional gas–solid two-phase system. Of note, these improved performances are attributed to the enhancement of the local surface plasmonic resonance of Cu@Ni nanoparticles by changing the local medium dielectric constant and prolonged carrier's lifetime originating from heterostructure. Moreover, plasmonic TiN nanoparticles play an important role in remaining the triphase interfacial system temperature at 90 °C and increasing methanol production excellently. While, the ionic liquid in the gas–liquid–solid system can activate CO2 molecules, thereby greatly improves the yield of methanol. In situ Fourier transform infrared (FTIR) spectra and 13C isotope labeling tests reveal the reaction path of CO2 on the photocatalyst surface. This work may provide a new direction for the efficient photoreduction of CO2 to methanol.

CAS / MDL: 6046-93-1 4766-57-8
研究领域: 化学 · 材料科学 · 环境科学 · 催化
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CARBOHYDRATE POLYMERS · 2023 · IF 11.2

Cellulose sulfate lithium as a conductive binder for LiFePO4 cathode with long cycle life

Xu Su,Han Fang,Hao Yang,Fangfang Zou,Gang Li,Lian Wang,Hongxin Liao,Wei Guan,Xuebu Hu

Polysaccharides can be potential binders for lithium-ion batteries due to their strong adhesion through numerous hydroxyl groups . As a novel waterborne lithiated polysaccharide derivative, cellulose sulfate lithium (CSL) is successfully synthesized and used as the binder for LiFePO 4 (LFP) cathode. The chemical structure of CSL is verified by FTIR-ATR, XRD, C 13 -NMR, GPC , EA , ICP and TGA . Compared to LFP cathode using polyvinylidene difluoride binder, electrochemical measurements show that the LFP cathode using CSL (LFP-CSL) has lower polarization and better rate performance owing to higher lithium-ion conductivity of CSL. The result of morphological analysis indicates that CSL binder can maintain an integrated LFP cathode structure during hundreds of cycles. As a result, the LFP-CSL cathode exhibits a discharge capacity of 133.4 mAh g −1 and maintains remarkable cycle stability with retention of 93.1 % after 300 cycles at 1C. These findings provide novel insights into the rational design of the binders for the LFP cathode.

CAS / MDL: 1310-66-3
研究领域: 材料科学 · 电化学 · 能源存储
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Chemical Engineering and Processing-Process Intensification · 2018 · IF 2.826

Preparation of Fe(III)-MOFs by microwave-assisted ball for efficiently removing organic dyes in aqueous solutions under natural light

Ding Chen,Peng-fei Feng,Fu-hua Wei

Fe-based metal-organic frameworks(Fe(III)-MOFs)were synthesized by Fe 2 (SO 4 ) 3 and trimesic acid using microwave-assisted ball milling method. The structure of the Fe(III)-MOFs was characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM) and Fourier transform infrared spectrometry (FTIR). The thermostability of the MOFs was analyzed by thermogravimetric analysis (TGA). Fe(III)-MOFs were added in aqueous solutions to remove organic dyes. The removal efficiencies of Orange II, CR and MB reached 95.9%, 98.7%, 95.7% respectively at 10℃ and reached 97.7%, 99.7%, 97.5% respectively at 35℃ in 300 min.

研究领域: 材料科学 · 环境科学 · 化学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Enhanced visible-light-driven photocatalytic activity of bi-phase titanium dioxide @ covalent organic framework Z-scheme system for photocatalytic removal of Cr (Ⅵ)

Yi Wen,Zheng Huang,Min Zhao,Longshan Zhao

The discharge of industrial heavy metal wastewater not only leads to environmental pollution, but also harms human health, so it is imperative to control heavy metal pollution. In the current work, a sequence of anatase/brookite TiO 2 @COF with different mass ratios, bi-phase TiO 2 and bare COF were successfully synthesized by simple hydrothermal synthesis. The photocatalytic activity of the prepared catalysts was assessed by reducing Cr(Ⅵ) in model pollutant (K 2 Cr 2 O 7 ). Under the condition of pH = 3, the Cr(Ⅵ) reduction rate of TiO 2 @COF-4 was as high as 99.19% in 30 min. The photocatalytic activity of TiO 2 @COF-4 remained stable in four consecutive cycles, suggesting that it has a potential application prospect for the removal of Cr(Ⅵ) in the actual environment. The morphology and structure of photocatalysts were observed by different techniques (SEM/EDS, HRTEM, BET analysis, XRD, FTIR and XPS). The specific reasons for the enhancement of photocatalytic performance of materials were explored by different methods (PL, UV–vis DRS, Mott-Schottky plots, I-T curves and EIS). Finally, we concluded that the photocatalytic system of TiO 2 @COF-4 may follow the typical direct Z- scheme mechanism. This work provides an effective solution for the water treatment of heavy metal pollution.

研究领域: 环境科学 · 材料科学 · 化学工程 · 纳米技术
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JACS Au · 2022 · IF 0

Plasma-Catalytic CO2 Hydrogenation over a Pd/ZnO Catalyst: In Situ Probing of Gas-Phase and Surface Reactions

Yuhai Sun,Junliang Wu,Yaolin Wang,Jingjing Li,Ni Wang,Jonathan Harding,Shengpeng Mo,Limin Chen,Peirong Chen,Mingli Fu,Daiqi Ye,Jun Huang,Xin Tu

Plasma-catalytic CO2 hydrogenation is a complex chemical process combining plasma-assisted gas-phase and surface reactions. Herein, we investigated CO2 hydrogenation over Pd/ZnO and ZnO in a tubular dielectric barrier discharge (DBD) reactor at ambient pressure. Compared to the CO2 hydrogenation using Plasma Only or Plasma + ZnO, placing Pd/ZnO in the DBD almost doubled the conversion of CO2 (36.7%) and CO yield (35.5%). The reaction pathways in the plasma-enhanced catalytic hydrogenation of CO2 were investigated by in situ Fourier transform infrared (FTIR) spectroscopy using a novel integrated in situ DBD/FTIR gas cell reactor, combined with online mass spectrometry (MS) analysis, kinetic analysis, and emission spectroscopic measurements. In plasma CO2 hydrogenation over Pd/ZnO, the hydrogenation of adsorbed surface CO2 on Pd/ZnO is the dominant reaction route for the enhanced CO2 conversion, which can be ascribed to the generation of a ZnOx overlay as a result of the strong metal–support interactions (SMSI) at the Pd–ZnO interface and the presence of abundant H species at the surface of Pd/ZnO; however, this important surface reaction can be limited in the Plasma + ZnO system due to a lack of active H species present on the ZnO surface and the absence of the SMSI. Instead, CO2 splitting to CO, both in the plasma gas phase and on the surface of ZnO, is believed to make an important contribution to the conversion of CO2 in the Plasma + ZnO system.

CAS / MDL: 10196-18-6
研究领域: 催化化学 · 等离子体化学 · 环境科学 · 可持续能源
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PROGRESS IN ORGANIC COATINGS · 2022 · IF 6.206

Synthesis and properties of photocurable polyurethane acrylate for textile artificial leather

Junxiang Ma,Kunyi Cai,Chao Yang,Meiqi Li,Xiaopeng Pan,Yi Huang,Juming Yao,Jinhuan Zheng,Jianzhong Shao

A new photocurable coating process that combines ultra violet light emitting diode (UV-LED) and deliberately synthesized photocurable polyurethane acrylate (PUA) was developed in this study. The structures of the PUA were characterized by attenuated total reflectance flourier transformed infrared (ATR-FTIR), porton nuclear magnetic resonance ( 1 H NMR) and gel permeation chromatography (GPC). The structure-activity relationship of such PUA was studied by rheological measurements, photopolymerization performance, and mechanical tests. By adjusting the molecular weight and the number of functional groups in the PUA, balanced the wear resistance and flexibility of the photocured coatings were achieved. The optimal formula for photocurable coating was obtained as follows: the R-value (the molar ratio of –NCO/–OH) of PUA was 1.3, the ratio of PUA/HEA (2-hydroxyethyl acrylate) was 60 wt%/40 wt%, and the ratio of end-capped agent HEA/PETA (pentaerythritol triacrylate) was 2/1. With the optimized photocurable coating formula, textile artificial leathers were fabricated and exhibited excellent colorfastness to rubbing, and Martindale abrasion resistance and satisfied fabric handle.

研究领域: 材料科学 · 高分子化学 · 纺织工程 · 涂层技术
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY · 2023 ·Vol. 332 ·期 1 ·23-32 · IF 1.6

Adsorption of uranium(VI) with a novel AMPS-modified thermostable β-cyclodextrin biosorbent

Ou Minrui,Li Wanying,Zhang Zihui,Xu Xiaoping

In this work, we synthesized a novel β -cyclodextrin/poly(2-acrylamide-2-methylpropionic acid)/attapulgite (CAMA) hydrogel for uranium(VI) adsorption. Various instrumental techniques such as FTIR, SEM, EDX, and TGA were utilized for characterization of the CAMA. Simultaneously, different important parameters, in specific pH, time, initial uranyl ion concentration and temperature were investigated to evaluate the optimal conditions of the adsorption process. The experiments proofs that the adsorption follows the pseudo-second-order kinetic model so as the Langmuir model, and revealed the maximum adsorption capacity of 434.78 mg g −1 at 298.15 K. Regeneration studies further sighted out the good reusability of the synthesized CAMA hydrogel.

CAS / MDL: 15214-89-8
研究领域: 环境科学 · 材料科学 · 化学工程
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Surfaces and Interfaces · 2023 · IF 6.2

Superior photocatalytic performance of ancillary-oxidant-free novel starch supported nano MFe2O4 (M = Zn, Ni, and Fe) ferrites for degradation of organic dye pollutants

A.V. Ravindra,M. Chandrika,Andem Sandeep

This work presents the effectual degradation of MB and MO dyes in an aqueous solution under UV light irradiation on nano ZnFe 2 O 4 , NiFe 2 O 4 , and Fe 3 O 4 without using any supplementary oxidants has been reported. Nano ZnFe 2 O 4 , NiFe 2 O 4 , and Fe 3 O 4 are successfully prepared via a co-precipitation technique utilizing biodegradable starch as a surfactant . XRD patterns reveal a pure spinel phase for all the samples. FTIR spectra confirm the successful embedding of the starch surfactant. SEM micrographs exhibit tiny spherical particles of size 5–8 and 4–6 nm for ZnFe 2 O 4 and NiFe 2 O 4 but spherical particles of 8–10 nm and flake-like particles of ∼14 nm thick for Fe 3 O 4 . N 2 sorption studies show type-IV isotherms typical of mesoporous structures. The direct bandgap of these ferrite nanoparticles is 2.03–2.15 eV, related to the metal D-d onsite transfers, which are permitted by spin but prohibited by parity. MB decolorization of 99% is achieved in less than 2 h for all the samples; in contrast, MO decolorization takes relatively longer irradiation. The decolorization kinetics suggests that the pseudo-second-order model is more appropriate to explain the decolorization process of MB and MO by the catalysts. The order of photocatalytic activity evaluated from rate constant (k 1 ) per SSA values is Fe 3 O 4 < ZnFe 2 O 4 < NiFe 2 O 4 for both MB and MO decolorization. NiFe 2 O 4 photocatalyst shows the best effect on the decolorization of both dyes due to its low bandgap and high surface area. All the ferrite catalysts demonstrate high stability with no substantial deterioration of photocatalytic activity even after three cycles. The results of this study endorse that the nano ferrites prepared in this work are potential candidates for the photocatalytic degradation of aqueous solutions of MB and MO.

研究领域: 环境科学 · 材料科学 · 化学
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PROGRESS IN ORGANIC COATINGS · 2024 · IF 6.5

Preparation of a bifunctional precursor with antibacterial and flame retardant properties and its application to cotton fabrics

Lifan Li,Xin Tang,Sha Zhou,Zaixing Zhang,Lingxiao Jing,Kun Luan,Zhaolong Su,Junjuan Huang,Tonghua Zhang

Cotton fabric is a cellulose-based material with complex capillary spaces, which enhance breathability and softness. However, these capillary spaces can promote bacterial growth with moisture during storage and daily use. Additionally, cotton fibers are highly flammable, posing a fire hazard to wearer. The lack of inherent antibacterial and flame retardant properties in cotton fabric limits its applications. In this paper, the triazole compound containing Schiff base (NABTA) was synthesized from 3-bromopropene, p-hydroxybenzaldehyde and 3-amino-1,2,4-triazole, followed by an addition reaction between Schiff base activity and 9,10-dihydro-9-oxa-10-phospha-phenanthrene-10-oxide (DOPO) to synthesize an antibacterial and flame retardant precursor (NABTA-DOPO). The structure of NABTA and NABTA-DOPO was characterized by FTIR and NMR. NABTA and NABTA-DOPO were applied to cotton fabrics to investigate and compare their antibacterial properties and thermal stability. The results showed that all the cotton fabrics treated with NABTA and NABTA-DOPO had favorable antibacterial effects. The introduction of DOPO had no significant effect on the antibacterial effect and mechanism of the fabrics. However, it otherwise improved the burning stability of treated cotton fabrics. The antibacterial activity of 10 g/L NABTA-DOPO treated cotton fabrics after chlorination against E. coli and S. aureus was over 99.99 %. The vertical burning test results showed that cotton fabrics treated with a concentration of 50 g/L NABTA-DOPO had improved flame retardant properties with a damaged length of 5.9 cm. In addition, the storage, washability, UV stability and antibacterial reproducibility experiments demonstrated the excellent durability and reproducibility of the N-halamine structure of chlorinated cotton fabrics. This study enhances cotton fabric by synthesizing and applying NABTA and NABTA-DOPO, resulting in improved multifunctionalities, including antibacterial properties, flame retardancy, UV resistance, and wettability.

研究领域: 材料科学 · 纺织工程 · 化学
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POLYMER DEGRADATION AND STABILITY · 2022 · IF 5.204

Engineering two nitrogen-containing polyhedral oligomeric silsesquioxanes (N-POSSs) to enhance the fire safety of epoxy resin endowed with superior thermal stability

Xinming Ye,Yu Feng,Panpan Tian,Zhimao Li,Yingchun Li,Wensheng Wang,Jie Li,Liang Qiao,Kun Wang,Wenchao Zhang,Ye-Tang Pan,Rongjie Yang

Despite remarkable advances in developing flame retardants and smoke suppressants for epoxy resin (EP), engineering nitrogen-containing polyhedral oligomeric silsesquioxane (N-POSS) to impart superior fire safety properties to EP has remained an intractable challenge. In this work, two nitrogen-containing polyhedral oligomeric silsesquioxanes (N-POSSs), namely, aminoethyl-aminopropyl-hepta-phenyl polyhedral oligomeric silsesquioxane (AEAP-POSS) and aminopropyl-hepta-phenyl polyhedral oligomeric silsesquioxane (AP-POSS), were synthesized through the “corner-capping” reaction. The molecular structures of N-POSSs were fully characterized by FTIR, 1 H NMR, 29 Si NMR and MALDI-TOF MS, and the synthesized AEAP-POSS and AP-POSS were introduced into EP to solve the shortcomings of flammability. TGA results showed that the incorporation of 4 wt% N-POSS nanoparticles distinctly improved the char residue at 800 °C, which significantly enhanced the thermal stability of the EP composites. When 4 wt% of AP-POSS was introduced into EP, reductions in the peak of heat release rate (p-HRR), fire growth index (FGI), peak of smoke production rate (p-SPR), and the peak of CO production rate (p-COP) reached to 60.6%, 70.2%, 52.3% and 60.4%, respectively. Subsequently, TG-FTIR and XPS were utilized to investigate the flame retardancy and smoke suppression mechanism. Our work presented a considerable advancement for the facile fabrication of flame retardants based on nitrogen-containing polyhedral oligomeric silsesquioxane compounds.

研究领域: 材料科学 · 化学工程 · 高分子科学 · 消防安全工程
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JOURNAL OF MATERIALS SCIENCE · 2023 ·Vol. 58 ·期 25 ·10359-10369 · IF 4.5

Reinforcing the mechanical properties of bamboo fiber/low density polyethylene composites with modified bamboo-woven structure

Liu Shujuan,Liu Lijuan,Yang Kangli,Yuan Zhiqing,Li Xinyi,Li Cancheng,Meng Shoutong

In order to improve the environmental problems caused by the extensive use of plastics, this paper introduced a new strategy to add and modify the physical structure, which could not only reduce the use of plastics, but also improve the mechanical properties of bamboo plastic composites. In this work, the bamboo-woven structure was introduced into the bamboo fiber/low density polyethylene (LDPE) composites to enhance the mechanical properties. Besides, to enhance the interfacial compatibility, maleic anhydride (MA) and polyvinyl alcohol (PVA) were used to modify LDPE and bamboo-woven structure, respectively. The mechanical properties of the prepared PVA-bamboo-woven structure/bamboo fiber/MA-LDPE composites were greatly improved. The bamboo plastic composites were characterized by Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy, water contact angle (WCA) test and mechanical property test. The results showed that the bamboo-woven structure/bamboo fiber/MA-LDPE composite has superior properties at 45% bamboo fiber content. The tensile strength reached to 33.842 MPa, which was increased by 65.01% compared to the bamboo fiber/MA-LDPE composites, and the bending strength reached to 36.6585 MPa increased by 81.46% in relation to the bamboo fiber/MA-LDPE composites. In addition, even a large number of hydrophilic bamboo fibers and bamboo-woven structure were carried by the composites, a good hydrophobicity was still maintained and the WCA reached to 93.71°. The composites with excellent mechanical properties and hydrophobicity provided a reference for the use of bamboo fibers in environmentally friendly packaging materials.

研究领域: 材料科学 · 高分子科学 · 环境工程 · 生物复合材料 · 机械工程
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