Molecular Catalysis
·
2023
·
IF 4.6
Tingting Pan,Yiming Tang,Yuxin Liao,Jiacheng Chen,Yaping Li,Jing Wang,Laisheng Li,Xin Li
Tetracycline antibiotics pose a significant threat to environmental sustainability and human health due to their high concentration in water and soil beyond safety limits. In this study, we developed a BiVO 4 photoelectrode modified with cobalt-phosphate cocatalyst hybrid nanocomposites to degrade tetracycline efficiently. The crystal structures of the composites and the chemical valence of the ions were characterized by X-ray diffraction (XRD) and X-ray photoelectron spectroscopy (XPS). The photocurrent generated from BiVO 4 /Co-Pi under visible light irradiation (λ ≥ 420 nm) was 1.99 mA/cm 2 , which was 10.5 times higher than that from pristine BiVO 4 film. The carriers’ dynamics were investigated by surface photovoltage spectroscopy (SPV) and transient photovoltage spectroscopy (TPV). BiVO 4 /Co-Pi demonstrated a 62.6% degradation rate of tetracycline within 60 min, which increased to 95.3% after adding peroxomonosulfate (PMS). Co-Pi cocatalyst facilitated charge separation and acted as the hole acceptor, thereby improving the degradation activity. Based on electron spin resonance (ESR) analysis, holes were identified as the dominant oxidizing species in the system. The activated Cobalt-phosphate cocatalyst along with the photogenerated-electrons facilitated the cobalt cycle process and generated sulfate radicals (•SO 4 − ) via PMS activation, leading to efficient tetracycline degradation.
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ULTRASONICS SONOCHEMISTRY
·
2023
·
IF 8.4
Jing Cui,Dan Fang,Xinquan Tian,Jun Peng,Di Chen,Shuangjiao Xu,Lei Ma
This study presents a novel approach for converting cottonseed hulls (CSHs) into valuable proanthocyanidins (PAs) through deep eutectic solvent (DES)-based ultrasound-assisted extraction (UAE-DES). Response surface methodology (RSM) was applied to optimize and model this process, resulting in maximum yields of 78.58 mg/g. The ideal PA extraction conditions were determined to be a liquid-to-material ratio of 36.25 mL/g, a water content of 33.21%, and an extraction period of 7.4 min. Molecular dynamic simulations (MDS) were performed to study the interactions between the solvent and target chemicals. Increased van der Waals forces and stronger interactions between DES and the target chemical catechin (CA) compared to those observed with methanol or water were observed. Furthermore, the optimized extract exhibited a higher PA content than can be obtained with conventional extraction methods and demonstrated antioxidant activity in vitro. The cottonseed hulls residues (CSRs) remaining after the extraction process can be used to produce activated carbon (AC CSR ), which has some capacity to adsorb methylene blue (MB) contaminants. This study offers a reference for the fruitful transformation of waste biomass into high-value products.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 52
·2305935
·
IF 19
Guoqiang Zhang,Wei Huang,Yangsen Xu,Yongliang Li,Chuanxin He,Xiangzhong Ren,Peixin Zhang,Hongwei Mi
Many cases of light absorption modification exceeding 700 nm or near-infrared (NIR) light are reported for capturing more than half of the solar energy, however, very few modifications can produce NIR photoactivity due to the inevitably introduced defects-induced non-radiative recombination. Here, taking four kinds of C/O co-doped red polymeric carbon nitride as examples, defect-repairing is carried out using alkali metal molten-salts (LiCl/NaCl and LiCl/KCl) or solid-salt (KCl) to activate their NIR photoactivity. The defect repair results from the passivation of alkali metal valence electron pairing and the formation of crystalline polyheptazine imide structure with more complete polymerization. More importantly, it sharply eliminates bulk defects (such as carbon vacancy and nitrogen vacancy) introduced by C/O co-doping. Since structural defects are inevitably introduced in most photocatalysts during expanding light absorption, this proposed strategy is bound to be universal in suppressing defects-induced non-radiative recombination to activate NIR photoactivity.
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ChemistrySelect
·
2023
·Vol. 8
·期 34
·e202301948
·
IF 2.1
Hai-Bo Wu,Xian-Tai Zhou,Xiao-Wu Zhou,Yan-Xiong Fang
Graphical Benzoic acid has been proved to be an efficient catalyst for the ring-opening polymerization of ϵ-caprolactone under mild conditions. A monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. It is expected to realize the one-step preparing of poly (ϵ-caprolactone) through the direct aerobic oxidation of cyclohexanone. The development of a feasible industrial method for poly(ϵ-caprolactone) (PCL) preparation is great of significant and challenging. The bulk ring-opening polymerization of ϵ-caprolactone (ϵ-CL) using various organic acid catalysts and benzyl alcohol (BnOH) as the initiator was developed. Benzoic acid (BA) has been proved to be an efficient catalyst for the ROP of ϵ-CL under mild conditions. The conversion of ϵ-CL to PCL was 84.7 % under the optimized reaction conditions, with number-average molecular weight ( M n ) and dispersity (PDI) of 7700 g/mol and 1.25, respectively. Moreover, a monomer-activated ring-opening polymerization mechanism mediated by benzoic acid was proposed. Overall, this work is expected to provide a feasible industrial method for the preparation of PCL using benzoic acid as organocatalyst.
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ACS Omega
·
2023
·
IF 4.1
Yunhui Liao,Feng Chen,Haishan Tang,Wubliker Dessie,Zuodong Qin
Aucubin (AU) is an active ingredient that exerts strong antioxidant and anti-inflammatory effects in the treatment of several diseases. In order to improve the efficiency of resource utilization of traditional biomass waste, Eucommia ulmoides seed-draff (EUSD) waste biomass was used as the raw material, and a series of deep eutectic solvents were selected to evaluate the extraction efficiency of aucubin from EUSD. A response surface experiment was designed based on a single-factor experiment to optimize the extract conditions. The results showed that the best conditions for aucubin extraction were an HBD–HBA ratio of 2.18, a liquid–solid ratio of 46.92 mL/g, a water percentage of 37.95%, a temperature of 321.03 K, and an extraction time of 59.55 min. The maximum amount of aucubin was 156.4 mg/g, which was consistent with the theoretical value (156.8 mg/g). Then, the performance of 12 resins for adsorption and desorption was contrasted. The results revealed that HPD950 resin exhibited the best performance, with an adsorption capacity of 95.2% and a desorption capacity of 94.3%. Additionally, the pseudo-second-order model provided the best match to the kinetics data, the Langmuir model provided the best fit to the isotherm data, and adsorption was a beneficial, spontaneous, exothermic, and physical process. In the recyclability test, the HPD950 resin had great potential and excellent sustainability in aucubin recovery. In the antioxidant activity study, the aucubin extract exerted a strong antioxidant ability with scavenging capabilities for four free radicals. Furthermore, the antifungal activity study found that the aucubin extract exhibited a good antifungal effect against 5 tested pathogens. The research results can provide a theoretical basis for the extraction of high-value components from waste biomass by deep eutectic solvent and a certain application value for the development and utilization of natural aucubin products.
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INTERNATIONAL JOURNAL OF ADHESION AND ADHESIVES
·
2023
·
IF 3.4
Wenxia Zhao,Xin Liu,Xuan Song,Caifang Zhang,Huaijun Chen,Xinwei Li,Kaihong Hui,Wei Zhao,Liang Qiao,Hao Zhu,Yi Cheng,Zenglin Wang
The purpose of this study was to enhance the adhesion strength between the epoxy resin (EP) substrate and the electroless copper plating layer by utilizing a MnO 2 –H 2 SO 4 –H 2 O–Na 4 P 2 O 7 system for surface modification. The effect of the volume ratio of V H2SO4 :V H2O and the duration of surface modification on various surface characteristics and adhesion strength was examined. The results provide valuable insights into the relationship between these factors and their impact on the properties of the surface. Optimal results were achieved with a volume ratio of V H2SO4 :V H2O at 3:1, a surface modification time of 20 min, Na 4 P 2 O 7 content of 30 g L −1 , and a modification temperature of 50 °C. Following the surface modification treatment, the EP substrate surface exhibited many deep micro-holes, significantly improving surface roughness . Due to the enhanced roughness on the surface and the application of suitable modifications, the contact angle on the EP substrate surface exhibited a significant decrease from 94.6° to 19.5°. This alteration caused the surface to transition from hydrophobic to hydrophilic . The adhesion strength between the EP substrate and the electroless copper plating layer was significantly increased to 0.74 kN m −1 . This improvement was attributed to the combined effects of surface roughness and hydrophilicity of the substrate surface.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2023
·
IF 4.2
Huangcong Tang,Jiayang Dou,Zhixian He,Jingwen An,Wenhuan Liu,Sheying Dong
Heterostructured catalysts with the potential synergies between the polymetallic sulfides and the construction of 1T-phase MoS2 are a promising alternative and contribute to obtain the enhanced hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) performance. Herein, the porous hybrid nanostructures coupling FeS2 and NiS complexes with 1T/2H phase MoS2 (FeNiSx@MoS2–HZHx) are prepared via a facile one-pot pyrolysis strategy accompanied by hydrazine hydrate (HZH)-induced phase transformation without the assistance of a template. The hybrid nanostructures possessing crystalline–amorphous (c–a) interface need overpotentials of 139 mV to achieve the current density of 10 mA cm–2 (η10) in 0.5 M H2SO4, which have superior kinetics for the HER process with a Tafel slope value of 57.9 mV dec–1. The 24 h continuous HER operated at η10 exhibits negligible deterioration, which has only a decrease of 3 mV at η10 after the 5000 cyclic voltammetry cycle tests, indicating the desirable stability of FeNiSx@MoS2–HZH2. Beyond that, the resultant FeNiSx@MoS2 requires 335 mV at η10. Specifically, the electrochemical and structural characterization prove that the enhanced HER performance is contributed from the incorporation of HZH to form FeS2/MoS2/NiS heterostructures and c–a interface sites coupling with 1T/2H phase MoS2, which provide more exposed active sites benefiting from the larger surface area. The simple and convenient design strategy has certain enlightenment for the development of sustainable energy production.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 31
·期 4
·6411-6424
·
IF 5.8
Li Yujia,Bi Erping
The interactions between organic pollutants and iron minerals play an important role in their environmental fate. In this study, the effects of low-molecular-weight organic acids (LMWOAs) on the adsorption and degradation of tetracycline (TC) on goethite were investigated. Tartaric acid (TA) was taken as the representative of LMWOAs to study the influencing mechanism through batch experiments and microscale characterization. In addition, the properties of TC-TA clusters under different pHs were determined by density functional theory (DFT) calculations. The results showed that all five LMWOAs inhibited TC adsorption and degradation. The preferential adsorption of TA on goethite changed TC adsorption from inner spherical to outer spherical complexation and mainly inhibited TC adsorption and degradation of the singly coordinated hydroxyl group. TC degradation rate decreased from 0.0287 to 0 h −1 in the first stage. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy results showed that TA could influence the interactions of amide groups, C = O on the A-ring, and dimethylamino group of TC with goethite, and the formation of ≡Fe(II) was inhibited. In addition to competing for the effective sites, the effects of complexation between TA and TC in solution should be considered. According to DFT calculations, hydrogen bonds could be formed between the carboxyl group of TA and the H atom of TC at different pH. These findings can provide evidence for estimating the contribution of adsorption and degradation to TC removal by iron oxides with the coexistence of LMWOAs in a soil–water environment. Graphical Abstract
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 13
·7862-7878
·
IF 4.22
Cao Xue-Fang,Yue Pan,Wei Qiu-Rui,Dang Yun-Fei,Zhang Si-Qi,Wei Zhi-Xian,Wang Rong-Zhen
In this study, a solar-driven photocatalyst La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) with p – n heterojunction structure was synthesized and characterized. The magnetic, photocatalytic properties, Fenton-like action and the synergistic effect of the photocatalysis and Fenton-like on methyl orange (MO) degradation of La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) were also investigated. Results show that p – n heterojunction was formed, and it has considerable photocatalytic properties under ultraviolet light and solar irradiation. More importantly, La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) also exhibits Fenton-like catalytic performance in the presence of H 2 O 2 and oxalic acid (OA). The main reactive radicals of the La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 –H 2 O 2 –OA–sunlight system are h + , · OH and · O 2 − . The chemical oxygen demand removal rate of MO wastewater in La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%)–H 2 O 2 –oxalic acid–sunlight system reached 72.4%; the value was higher than that of the sum of single photocatalysis (34.5%) and Fenton-like-dark system (27.6%), indicating that there is a synergistic effect between the photocatalysis and Fenton-like on MO degradation. In addition, La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) displays approximately superparamagnetism and has higher saturated magnetization ( M s ), low coercive force and residual magnetism. So it can be easily recovered by an external magnetic field and can be reused 6 times. It was anticipated that La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) with p – n heterojunction structure is a stable and reusable solar-light-driven magnetic photocatalyst and has great potential applications for wastewater treatment. Graphical abstract The magnetic La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) with p – n heterojunction structure was synthesized and characterized by different methods. The magnetic, photocatalytic properties, Fenton-like action and the synergistic effect of the photocatalysis and Fenton-like on methyl orange (MO) degradation of La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%) were also investigated. It is not only a solar-driven photocatalyst with high efficiency, but also shows excellent Fenton-like catalytic effect. And the photocatalysis and Fenton-like system exhibited synergetic catalytic effect on MO degradation by La 0.7 Sr 0.3 MnO 3 /α-Fe 2 O 3 (20%). Furthermore, near superparamagnetic characteristics of the catalyst make it easy to recycle by the external magnetic field and can be reused for 6 times, suggesting that it is a stable multifunctional catalyst.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Tingting Liu,Sheng Cai,Genfu Zhao,Zhihui Gao,Shuming Liu,Huani Li,Lijuan Chen,Mian Li,Xiaofei Yang,Hong Guo
Along with the continuous consumption in lithium-ion batteries (LIBs), the price of cobalt is inevitably going up in recent years. Therefore, recycling valuable Co element from spent devices, and boosting its service efficiency are becoming two indispensable approaches to promote the utilization of Co in various energy conversion/storage devices. Herein, we realize the recovery of Co from spent LIBs and synthesize a three–dimensional (3D) sea-urchin-like cobalt nitride composite material (labeled as CoN-Gr-2), which is used as a bi-functional catalyst for water splitting. Benefiting from the intrinsic high conductivity, larger surface area and unique 3D sea–urchin–like architecture, CoN-Gr-2 shows an excellent electron transfer efficiency, highly exposed active sites as well as the superior mass transport capacity. The CoN-Gr-2 catalyst exhibits low overpotentials of 128.9 mV and 280 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), which are comparable to the commercial 20 wt% Pt/C and RuO 2 catalysts. Moreover, when adopting CoN-Gr-2 as both anode and cathode materials for overall water splitting (in 1.0 M KOH electrolyte), the assembled cell achieves a current density of 10 mA cm −2 at 1.61 V, which almost close to that of Pt/C||RuO 2 benchmark (1.60 V), demonstrating its superior water-splitting efficiency. Meanwhile, the CoN catalysts exhibit strong chemical interaction with the Gr support, suppressing the aggregation of CoN catalysts and maintains their high activity during HER and OER reactions. So, the cell exhibits a high current retention of 97.3% after 40 h. This work successfully develops an industrial chain from recycling Co wastes in spent energy devices to controllably designing 3D sea-urchin-like CoN-Gr with high water splitting efficiency. Therefore, it could further promote the efficient utilization of valuable Co element in various energy devices.
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MOLECULES
·
2021
·Vol. 26
·期 8
·2208
·
IF 4.412
Muhammad Sajid,Muhammad Rizwan Dilshad,Muhammad Saif Ur Rehman,Dehua Liu,Xuebing Zhao
Furfural is one of the most promising precursor chemicals with an extended range of downstream derivatives. In this work, conversion of xylose to produce furfural was performed by employingp-toluenesulfonic acid (pTSA) as a catalyst in DMSO medium at moderate temperature and atmospheric pressure. The production process was optimized based on kinetic modeling of xylose conversion to furfural alongwith simultaneous formation of humin from xylose and furfural. The synergetic effects of organic acids and Lewis acids were investigated. Results showed that the catalystpTSA-CrCl3·6H2O was a promising combined catalyst due to the high furfural yield (53.10%) at a moderate temperature of 120 °C. Observed kinetic modeling illustrated that the condensation of furfural in the DMSO solvent medium actually could be neglected. The established model was found to be satisfactory and could be well applied for process simulation and optimization with adequate accuracy. The estimated values of activation energies for xylose dehydration, condensation of xylose, and furfural to humin were 81.80, 66.50, and 93.02 kJ/mol, respectively.Keywords:catalysis;chlorides;furfural;kinetics;lewis acid;p-toluenesulfonic acid;xylose
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2021
·
IF 4.098
Yan Guo,Huihui Wang,Zhenjia Chen,Xu Jing,Xiaowen Wang
A deep eutectic solvent (DES)-based extraction method is established to facilitate the determination of methomyl in grain via enzyme inhibition fluorescence. The environmentally-friendly DES was synthesized from proline and ethylene glycol and used as a green replacement for traditional extraction solvents that are generally toxic. The DES was added to grain samples and vortex extraction of methomyl, the supernatant was then collected for fluorescence detection. Biomass carbon quantum dots (CQDs) synthesized from millet were used as fluorescent probes. Acetylcholinesterase catalyzes the hydrolysis of acetylthiocholine iodide to thiocholine. The positively-charged thiocholine interacts electrostatically with the negatively-charged quantum dots resulting in the quenching of their fluorescent emission. The pesticide extract solution blocks the enzyme activity and thus recovers the fluorescent from the quantum dots. The fluorescence response was correlated with the amount of methomyl residue in the grain over the range 0.01 to 5 mg kg −1 . The limit of detection was found to be 0.003 mg kg −1 , and the limit of quantification 0.01 mg kg −1 . Recoveries of 86.5% to 107.8% were obtained using real samples, including millet, rice, wheat, and barley, with a relative standard deviation of less than 3.8%. The method is efficient and convenient and has good application prospects for extracting and detecting pesticides in grain samples.
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