ACS Omega
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2023
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IF 4.1
Daniu Cai,Guangcai Zhang,Dongliang Hu,Jianyang Li,Minggong Wang,Yingwu Zhang,Junsheng Yuan
For the separation of metal ions, ionic liquid-based aqueous biphasic systems (IL-ABSs) offer a promising alternative to solvent extraction. However, the incorporation of an extensive quantity of inorganic salts restricts their practical application. Because heavy metal wastewater often contains high concentrations of inorganic salts, it offers good prospects for the application of IL-ABSs in the separation of heavy metals. In this work, an IL-ABS was formed by tributyltetradecylphosphonium chloride ([P44414]Cl), and simulated high-salinity wastewater (NaCl and Na2SO4 as the main inorganic salts) was used for the separation of heavy metals. The phase diagram results indicated that the formation of a two-phase system required a relatively high salt concentration. The extraction process followed the mechanism of anion exchange; thus, heavy metals such as zinc and cadmium that formed complexes with chloride ions could be effectively extracted (extraction rate >99.5%) with a very fast rate (extraction time <1 min) at a wide pH range (pH = 2–7). After extraction, the metals could be stripped well (stripping rate >99.5%) after contact with the NaOH solution. This research provided a new approach for treating heavy metals in high-salinity effluents, which has the advantages of IL-ABS and avoids the disadvantages of adding large amounts of inorganic salts at the same time.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yangzhi Xu,Zirui Gao,Yao Xu,Xuetao Qin,Xin Tang,Zhiwei Xie,Jinrong Zhang,Chuqiao Song,Siyu Yao,Wu Zhou,Ding Ma,Lili Lin
Hydrogenation of CO 2 into methanol at low-temperature on Cu-based catalysts is of great significance, but remains challenging to enhance activity. In this paper, we report an inverse catalyst constructed with nano-ZrZnO x supported on Cu particles with outstanding methanol synthesis performance at 220 ℃, two times higher than that of commercial Cu/ZnO/Al 2 O 3 catalysts under the same conditions. Detailed structure characterization and performance evaluation demonstrate that the ZrZnO x mixed oxide serves as the most active oxide-metal interface site for CO 2 hydrogenation. The ZrZnO x /Cu inverse catalyst increases the weak and medium CO 2 adsorption sites which are further demonstrated responsible to the methanol productivity. In situ DRIFTs studies reveal that the inverse interface accelerates the reduction of asymmetric formate intermediates and prevents the generation of CO. The combination of enhanced CO 2 activation capability and accelerated hydrogenation rate of intermediates over the ZrZnO x /Cu inverse catalyst probably contribute to the remarkable methanol synthesis performance from CO 2 .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2023
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IF 4.2
Erhu Li,Xuliang Lin,Shirong Sun,Xueqing Qiu
The highly selective conversion of technical lignin to low-oxygen-content compounds is still challenging due to the presence of methoxy and ether bonds in natural lignin. Herein, tunable ternary deep eutectic solvents (DESs) containing choline chloride, oxalic acid, and another bifunctional reagent with a hydrogen-bond donor and nucleophilic function were used for the β-aryl ether bond cleavage or Cα-etherification of lignin followed by pyrolysis to improve the yield of methoxy-free lignin monomers. The relationship between the lignin structure and pyrolysis behavior was investigated by 2D-NMR, FTIR, GPC, XPS, TGA, TG-FTIR, EPR, etc. The DES pretreatment changed the pathway of lignin pyrolysis toward a higher yield of bio-oil and methoxy-free products. Compared with technical lignin, the yield of phenolic products after Cα-etherification with ethanol and ethylene glycol as nucleophilic reagents increased from 0.73 × 1011 to 4.10 × 1011 and 5.56 × 1011 area/mg, respectively. Besides, the introduction of ethanol and ethylene glycol is more conducive to the demethoxylation of pyrolysis products and the formation of methoxy-free phenols during pyrolysis. This work realizes the conversion of lignin to high-value phenolic products with low-oxygen-content compounds without adding catalysts by a pyrolysis strategy.
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Food Bioscience
·
2023
·
IF 5.2
Shijin Xiong,Dandan Qiu,Xiaoyan Xu,Tonghao Du,Zhen Peng,Muyan Xiao,Tao Huang,Jinqing Huang,Hongbing Ren,Mingyong Xie,Tao Xiong
Laotan Suancai is a well-known Chinese traditional fermented vegetable with a unique flavor. However, there are significant differences in the quality of Laotan Suancai pickled by jars (LTSC-J) and pools (LTSC-P) on an industrial scale. To reveal the effect of fermentation craft on Laotan Suancai quality, the microbial community, flavor metabolites, and physicochemical properties of the two types of Laotan Suancai, as well as their interrelationship were investigated. LTSC-P had higher salinity, glucose content, and histidine content, while LTSC-J had higher TA, lactic acid content, and isobutyric acid content. Nine differential aroma-active compounds were found between the two types of Laotan Suancai: anethole , eucalyptol, diallyl sulfide, estragole, diallyl disulfide , eugenol, linalool, nonanal , and ethyl butyrate. LTSC-P showed a higher relative abundance of Weissella , Acinetobacter , Pseudomonas , Allorhizobium-Neorhizobium-Pararhizobium-Rhizobium , Inhella , and Leuconostoc compared to LTSC-J. Co-occurrence analysis indicated the distinct differences in the co-occurrence patterns of the microbial network across the two types of Laotan Suancai. RDA analysis indicated that glucose, salinity, TA, maltose , and nitrite were the main drivers for the differences in bacterial communities between the two types of Laotan Suancai. Spearman correlation analysis revealed strong correlations between 18 bacteria and 61 flavor compounds. Finally, bacterial metabolic function prediction indicated that sulfide and aromatic ester may be biosynthesized by sulfur metabolism , cysteine and methionine metabolism, pyruvate metabolism, and butanoate metabolism. Overall, these findings provide important guidance for improving the manufacturing and quality of Laotan Suancai.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Zhen Song,Jiahui Chen,Hao Qin,Zhiwen Qi,Kai Sundmacher
Although eutectic solvents (ESs) have received considerable attention as sustainable process fluids for various applications, discovering novel ESs remains challenging as computational methods for predicting the formation of eutectics are still scarce. In the present work, both the original and modified UNIFAC models are evaluated and extended for predicting the solid–liquid equilibria (SLE) of ES systems. The applicability of the two versions of UNIFAC models is first evaluated based on the SLE of 25 ES systems composed of only conventional components. Motivated by the good evaluation results, the SLE of 50 ES systems involving one salt component are employed to extend the UNIFAC models to include novel salt-component-related functional groups. The obtained models cover widely-reported salt components of choline/tetraalkylammonium chloride/bromide and conventional components of fatty alcohols and fatty/dicarboxylic/α-hydroxy acids. A theoretical design of novel ESs in a large scale is performed with the best-performing model extension, wherein four designed ES systems are validated experimentally.
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MATERIALS CHEMISTRY AND PHYSICS
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2023
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IF 4.6
Debin Zeng,Longtao Wang,Ruian Du,Zhen Wu,Xiting Wang,Chunguang Kuai,Yuzheng Guo,Changlin Yu
CO 2 photoreduction under mild conditions remains challenging, attributing to sluggish kinetics of complex coupling process of multi-electrons-protons and inefficient electron-hole pairs utilization. Herein, with Zn 3 V 2 O 8 as a phase transformation material, we construct an effective Zn 2 V 2 O 7 /Zn 3 V 2 O 8 /ZnO (OVZn) Z-scheme system by partial decomposition of Zn 3 V 2 O 8 into Zn 2 V 2 O 7 and ZnO. Time-resolved fluorescence decay (TRFD) spectra investigation shows that the photogenerated electrons of Zn 2 V 2 O 7 and ZnO recombine with the holes of Zn 3 V 2 O 8 , retaining more reductive electron of Zn 3 V 2 O 8 for CO 2 reduction. Moreover, in-situ Fourier-transform infrared spectroscopy suggests that the heterostructure can lower the energy barrier of CO desorption by changing bridge-bonded CO to linear-bonded CO and optimizing the energy barrier of CO production. Moreover, Cu, Ag and Au loading on OVZn greatly enhance light harvesting and promote photoelectric conversion, producing much photogenerated electron-hole pairs for CO 2 reduction. OVZn and metal loaded OVZn have better photocatalytic performance, showing application superiority on CO 2 photoreduction.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Chen,Xiaona Dong,Ruonan Feng,Wanying Li,Dahu Ding,Tianming Cai,Canlan Jiang
Triclosan (TCS) is a compound in pharmaceutical and personal care products (PPCPs) that preferentially accumulates in soil and may threaten human health. Iron-based persulfate activation processes (Fe-PAPs) are a promising technique in soil remediation but are limited by their narrow pH application range and resultant iron precipitation. In this study, oxalic acid (OA) was specifically introduced to improve the efficiency of Fe 2+ -activated persulfate (PS) processes for TCS degradation in soil. The complexation of OA and Fe 2+ improved the total iron concentration in the Fe 2+ /OA/PS system and prevented iron precipitation. Fe-minerals in soil were also dissolved by OA, which participated in PS activation. The most appropriate proportion of Fe 2+ /OA/PS is 1:1:1, and approximately 85% of the TCS was degraded within 240 min compared with 45% in the Fe 2+ /PS system. SO 4 • - and 1 O 2 played important roles on TCS oxidation, while O 2 • - and CO 2 • - mainly participated in the iron cycle. The weak stretch of Fe-O in OA containing treatments in ATR-FTIR measurements provided evidence that OA dissolved the Fe-minerals. The introduction of OA in the Fe 2+ /PS system in four different soils reduced the negative effect of soil organic matter on TCS degradation. Three types of intermediates including hydroxylation, cleavage of ether bonds and cyclization products, were identified by LC-Q-TOF-MS. Column experiments were used to study the feasibility of in situ chemical oxidation (ISCO) remediation of TCS in the Fe 2+ /OA/PS system. Our findings indicated the ability of OA to be used as a cheating agent in Fe-PAPs for TCS soil remediation.
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Journal of Water Process Engineering
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2023
·
IF 7
Jueqin Chen,Cao Yang,Tian Wu,Jian Wang,Lihui Yang,Wei Sun,Wei Li,Anqi Wang,Sihao Lv
At present, considerable efforts have been devoted to the development and application of MOFs, and some MOFs have realized industrial mass production and sales. However, little attention was paid to the treatment and disposal of the resulting waste MOF . In this study, the antibiotic(N source)-saturated waste MOF adsorbent was recycled into metal-free N-doped carbocatalyst through one-step pyrolysis . Compared with the pristine MOF-derived undoped carbon, N-doping led to nearly 2-fold enhancement in the pseudo-first-order rate constant for catalytic ozonation of oxalic acid (OA), and the COD removal of coking and swine wastewaters reached more than 60 % within 30 min. Apart from the formation of spongy porous morphology and the boosting of specific surface area from 253.7 to 320.6 m 2 /g after N doping, the characterization analysis and OA degradation results revealed that oxygen vacancies, hydroxyl groups and N species were the main active sites. Furthermore, it was identified the dominant contribution of OH in OA destruction, followed by O 2 — and 1 O 2 , and the metal-free N-doped carbon displayed good reusability and chemical stability. This study proposes a feasible strategy for the utilization of waste MOF, showing great reference significance for the expansion of material functions.
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LWT-FOOD SCIENCE AND TECHNOLOGY
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2023
·
IF 6
Qi Chen,Ying Li,Kangling Yan,Guanghui Li,Donghui Luo,Weidong Bai,Xiaofang Zeng,Qingping Wu,Jinhua Deng,Hao Dong
Chaozhou pickle, a traditional Chinese fermented vegetable product, is highly regarded among consumers due to its unique flavor. This work monitored the flavor substances and microbial communities of Chaozhou pickles during fermentation by gas chromatography-ion mobility spectrometry (GC-IMS) and high-throughput sequencing. A total of 70 volatile compounds were identified from Chaozhou pickles. In addition to fruit aroma esters, the pickles also contain aldehydes, ketones, alcohols, acids, and heterocyclic compounds. The four pickles exhibited a prevalence of Cyanobacteria, Proteobacteria, and Firmicutes as the leading bacterial phyla , while Weissella, Leuconostoc, and Lactobacillus were identified as the predominant bacterial genera. Physiochemical quality and acid properties of Chaozhou pickle were also investigated. Results revealed a significant reduction in hardness, chewiness and pH during fermentation, as well as a notable increase in free amino acids, and organic acid levels. These results could contribute to a greater comprehension of the role of microorganisms in flavor formation during fermentation and provide a scientific foundation for the industrialization of Chaozhou pickle.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
·
2023
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IF 4.4
Zhen Lin,Chuangui Cai,Wei Chen,Qian Deng,Jialin Yang,Kaiyuan Huang,Haohua Deng,Xinhua Lin,Wei Chen,Wensong Yao
Chemiluminescence (CL) intensity of luminol-H 2 O 2 system was dramatically enhanced by cetyltrimethylammonium bromide (CTAB) micelle-mediated 6-aza-2-thiothymine-protected gold nanoclusters (ATT-AuNCs). It is proved that spherical micelles of CTAB in aqueous solution improved the dispersity of ATT-AuNCs, thus enhancing their catalytic activity, which brought in the increased CL intensity of luminol-H 2 O 2 system. Carbazochrome sodium sulfonate (CSS) with a hemostatic containing tetrahydroindole structure broke the spherical micelles and notably quenched the CL intensity of luminol-H 2 O 2 -CTAB-ATT AuNCs system. Based on these results, a simple, fast, and sensitive CL method has been developed for the detection of CSS with a linear range of 0.25–25 μM and a detection limit of 0.11 μM. The method has also been successfully applied to the determination of CSS in serum with satisfied recoveries in the range of 89.6 % to 103.7 %. This study not only provides an effective approach for CSS detection but also paves the way for AuNCs-based CL applications.
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CHEMOSPHERE
·
2023
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IF 8.8
Tianyuan Xu,Ting Chen,Zhenhua Chen,Yijun Cao,Yaowen Xing,Xiahui Gui
A photochemical system combining iron (hydr)oxides and oxalate (Ox) shows application prospects in wastewater treatment due to the abundance of reactive oxygen species (ROS) generation. Nevertheless, it is a challenge to the investigate photochemical activity of iron (hydr)oxides/Ox systems with varying structural properties. Herein, the photochemical behaviors of Ox on goethite (Gt) surface from the view of structural dependent activity, containment degradation, and ROS generation were explored in detail. Results confirmed that bidentate mononuclear was formed on Gt surface after complexing Ox. Combined with density functional theory calculation and pH time evolution during aniline degradation, the photochemical activity of the Gt/Ox system fell in between that of ferrihydrite/Ox and hematite/Ox systems. After irradiating 120 min visible light, 96.5% aniline was degraded by 1.0 mM Ox and 0.2 g/L Gt. The amount of •OH in vis/Gt/Ox system could be up to 309.3 μM and its generation was closely associated with Fe(II) while slightly affected by the generated H 2 O 2 . Moreover, as revealed by high-performance liquid chromatography with mass spectrometric and Ecological Structure Activity Relationships software, the toxicity of the intermediates of aniline degradation in the vis/Gt/Ox system towards fish and green algae increased first but then declined accompanied by the generation of non-toxic ring-opening products at the end of reaction. According to the findings in the presented study, it could be concluded that vis/Gt/Ox is a promising approach to wiping out aniline wastewater.
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高影响因子
Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Hu Changjiang,Jiang Zhiwen,Wu Qunyan,Cao Shuiyan,Li Qiuhao,Chen Chong,Yuan Liyong,Wang Yunlong,Yang Wenyun,Yang Jinbo,Peng Jing,Shi Weiqun,Zhai Maolin,Mostafavi Mehran,Ma Jun
The efficient use of renewable X/γ-rays or accelerated electrons for chemical transformation of CO 2 and water to fuels holds promise for a carbon-neutral economy; however, such processes are challenging to implement and require the assistance of catalysts capable of sensitizing secondary electron scattering and providing active metal sites to bind intermediates. Here we show atomic Cu-Ni dual-metal sites embedded in a metal-organic framework enable efficient and selective CH 3 OH production (~98%) over multiple irradiated cycles. The usage of practical electron-beam irradiation (200 keV; 40 kGy min −1 ) with a cost-effective hydroxyl radical scavenger promotes CH 3 OH production rate to 0.27 mmol g −1 min −1 . Moreover, time-resolved experiments with calculations reveal the direct generation of CO 2 •‒ radical anions via aqueous electrons attachment occurred on nanosecond timescale, and cascade hydrogenation steps. Our study highlights a radiolytic route to produce CH 3 OH with CO 2 feedstock and introduces a desirable atomic structure to improve performance.
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危险品化学品经营许可证（带存储）