CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yong Yang,Xinxin Ma,Zifen Li,Yanru Wang,Chao Ju,Lidong Cao,Yongquan Zheng,Qingming Zhang
Neonicotinoids, ones of the most used pesticides extensively present in water environment, are hazardous to environment and human. Herein, a novel magnetic adsorbent ZIF-8-HA@MCSB is designed by modifying ZIF-8 and humic acid (HA) onto the surface of magnetic corn stalk biochar (MCSB) for removing imidacloprid (IMI) and thiamethoxam (THI) from water. MCSB has a superior adsorption performance among magnetic biochars (MBCs); the modification of ZIF-8 creating hierarchically porous structure and HA promoting the crystal growth of ZIF-8 can enhance its adsorption performance. Hence, ZIF-8-HA@MCSB exhibits the high maximum adsorption capacities for IMI (163.9 mg g −1 ) and THI (123.5 mg g −1 ). Meanwhile, the HA modification offers a protective shell for magnetic Fe 3 O 4 , which endows ZIF-8-HA@MCSB with distinguished magnetic stability. Even in pH = 2 solution, ZIF-8-HA@MCSB still possesses a saturation magnetization value of 13.07 emu g −1 , which is beneficial for its separation and reuse. Especially, ZIF-8-HA@MCSB can be repeatedly used 5 times with high removal efficiencies (over 90%). Furthermore, the low Fe (less than 0.3 mg L −1 at pH ≥ 2) and Zn (less than 1.0 mg L −1 at pH ≥ 3) leaching concentrations in a wide pH range guarantee the environmental security of ZIF-8-HA@MCSB. And a promoting effect on wheat growth enables waste ZIF-8-HA@MCSB potentially to be fertilizer for crop production, which agrees with the sustainable concept. Therefore, the advantages of having high adsorption capacities for IMI and THI, resistant to acid, and friendliness to environment indicate that ZIF-8-HA@MCSB has a significant potential for real neonicotinoids removal. Novelty Statement In this work, a novel magnetic adsorbent (ZIF-8-HA@MCSB) with the high adsorption capacities of IMI and THI is obtained by simply modifying ZIF-8 and humic acid (HA) onto the magnetic corn stalk biochar (MCSB) surface. Such a magnetic adsorbent has never been reported before. More importantly, compared with various modification methods to increase the adsorption capacity, there are few reports on concerning the acid resistance and environmental friendliness of magnetic adsorbents, especially the corresponding adsorption capacity also increases.
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CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Xinrong Ke,Ping Lu,Jinling Cai,Jiayuan Wang,Changshen Ye,Chen Yang,Ting Qiu
The removal of aromatic sulfur-containing species by adsorption method in liquid hydrocarbon fuels (LHFs) are concerned in worldwide, but it is still a challenge due to intricacy-designed adsorbents, resulting in high cost of preparation and poor stability. Herein, an easy-prepared adsorbent, Zn-NC-T (T represents the carbonization temperature, T = 600, 800 and 1000 °C), which derived from the carbonization of low-cost ZnCl 2 -chitosan polymers, is reported. The optimal Zn-NC-800 exhibits dibenzothiophene (DBT) uptakes of 43.3 mg S/g, which is superior to many reported desulfurization adsorbents, including metal–organic frameworks, zeolites and metal-loaded porous carbons. It also keeps satisfactory reusability with adsorption capacity loss of 5.3 mg S/g after 5 cycles because of the high-efficiency removal of adsorbates under high temperature regeneration. Moreover, the Zn-NC-800 shows great potential for sulfur-free LHFs production in the industry by breakthrough experiment for adsorbing low-concentration DBT (100 ppm w S) with ca. 0 ppm w S content in outlet LHFs. And the mechanism investigation on the adsorption isotherms and kinetics indicates that the adsorption process of DBT is controlled by chemisorption. Furthermore, DFT calculations suggest that the Zn, N-co-doped carbons show stronger adsorption strength (e.g., DBT, −1.79 eV) than the sole N-doped carbons (−0.93 eV), indicating the main contribution of Zn, N-cooperated adsorptive sites. The reported Zn-NC-T equips with advantages of low-cost raw materials, high adsorption capacity and good reusability, making it promising candidate for production of sulfur-free LHFs.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Erjian Huang,Yueyang Xu,Yachun Ren,Peng Zhang,Yongping Zeng
Faujasite (FAU)-type zeolites are promising adsorbents for the removal of sulfides from fuels, but their micropores are not capable to accommodate the large-sized thiophenic compounds. FAU zeolites (NaX and NaY with the low and high Si:Al ratios, respectively) with hierarchical micro/mesoporous structures were synthesized by sequential acid-base treatment to enhance the adsorption capacity and reduce the limitations of diffusion for the sulfides. To further to improve the desulfurization performance, the hierarchical structure of FAU zeolites containing Cu + were prepared by ion-exchange and methanol vapor-induced reduction methods at a relatively low temperature (473 K). For the large-sized benzothiophene , both the HP-Cu(I)Y and HP-Cu(I)X zeolites with mesopores have a very high adsorption capacity, reaching 51.8 mg S/g and 56.1 mg S/g, respectively. In addition, the results show that HP-Cu(I)X has a higher adsorption capacity than that of some other FAU-type adsorbents reported.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2022
·
IF 3.656
Fangli Yi,Qing Yang,Xinyu Li,Yiqi Yuan,Hongmei Cao,Kewei Liu,Hongjian Yan
Donor–acceptor domains hold the key to tailoring photochemical properties and charge carrier mobility of conjugated microporous polymers (CMPs) for application in photocatalytic water splitting. Herein, a family of electron-withdrawing 1,3,5-triazine and electron-donating fused thiophene based porous polymers are obtained via C–H arylation . The TBT-BDT showed an excellent HER of 4238 μmol g −1 h −1 , which is 17-fold and 3-fold higher than that of TBT-Th and TBT-TT, respectively. In addition, TBT-BDT facilitates overall water splitting to produce stoichiometric amounts of H 2 (28 μmol g −1 h −1 ) and O 2 (14 μmol g −1 h −1 ). The significant difference in the photocatalytic performance was mainly ascribed to the band structure change of the polymers, which underlined the importance of the donor unit on the performance of D−A type photocatalysts and indicated that thiophene-contained unit BDT is an excellent donor for high photocatalytic activity .
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2022
·
IF 5.895
Tong Zhou,Xue Xia,Heping Cui,Khizar Hayat,Xiaoming Zhang,Chi-Tang Ho
The intervention of cysteine (Cys) on the formation of 2,3-butanedione and pyrazines was evaluated during the thermal processing of the alanine-xylose Amadori compound (AX-ARP). With the involvement of Cys, the competitive formation of 2,3-butanedione and pyrazines was induced. The formation of 2,3-butanedione in the AX-ARP/Cys model was suppressed due to the inhibitory effect of the precursors of 2,3-butanedione like deoxypentosones, while the added Cys in the AX-ARP/Cys model competed with the recovered alanine (Ala) to capture glyoxal and methylglyoxal to make up for the absence of pyrazines in the AX-ARP model at an initial pH value of 7. The content of pyrazines increased from 0 up to 16.48 μg/L (120 °C, 120 min). Exogenous Cys itself showed lower reactivity with 2,3-butanedione through the Strecker degradation reaction; while the pH was increased to 8, the degradative products of Cys were facilitated to consume the residual 2,3-butanedione giving rise to the formation of 2,4,5-trimethylthiazole at 120 °C. It was the degradative products of Cys that accelerated the reaction for consumption of 2,3-butanedione rather than Cys itself. Additionally, the inhibitory effect of Cys on 2,3-butanedione formation was weakened under a basic condition, while the promotional effect on the formation of pyrazines was further boosted. With more Cys participating in the process of AX-ARP thermal degradation, the formation of 2,3-butanedione was further inhibited, while the yields of pyrazines were increased.
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Journal of Cleaner Production
·
2023
·
IF 11.1
Yulin Zhang,Guozhao Ji,Fahim Ullah,Aimin Li
The properties of tire pyrolysis oil are similar to diesel oil, but the high sulfur content in the pyrolysis oil limits its use in diesel engines . In this work, taking the boiling point range of traditional diesel oil as the cutting temperature, a fraction in the temperature range of 190–350 °C was obtained by distillation of tire pyrolysis oil (TPO 190–350 °C ). The sulfides in TPO 190–350 °C are mainly benzothiophene derivatives. And a simple and effective POM-based catalyst ([C 16 H 33 N(CH 3 ) 3 ] 3 PW 4 O 24 ) has been used in the oxidation desulfurization process for the removal of sulfur compounds from the oil. The catalyst played the role of transferring reactive oxygen species atoms on H 2 O 2 to sulfur compounds . The benzothiophene , dibenzothiophene , and 4,6-dimethyl-dibenzothiophene (500 ppm S) in model oil could be converted to the corresponding sulfone within 1 h at 40 °C. Even if the sulfur content was increased to 2000 ppm, the catalyst exhibited well catalytic performance under the same conditions. The catalyst could be recycled and reused with no loss of desulfurization efficiency. Distillation could effectively reduce the presence of olefins in the oil leading to reduce oxidation performance during the oxidation desulfurization process (ODS). In the subsequent desulfurization experiments of TPO 190–350 °C , a high desulfurization efficiency (91.28%) was achieved for TPO 190–350 °C , with initial sulfur contents of 11033 ppm declining to 961 ppm.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2023
·
IF 3.9
Wanyi Tao,Bo Zhang,Luxia Yin,Xiao Teng,Zhang Wen,Zekai Zhang,Wensheng Ning
Fabrication of adsorbent can play an important role in the adsorption desulfurization technology as a most promising deeply desulfurization technology. Ag 2 O/CeO 2 /SiO 2 aerogel composites were synthesized, where the easy oxidation of Ce 3+ into Ce 4+ was realized by adding hydrogen peroxide, and were utilized to remove thiophenics from model fuels and aromatics. Compared with Ag 2 O/SiO 2 and CeO 2 /SiO 2 , the adsorption uptake and solvent washing regeneration performance of Ag 2 O/CeO 2 /SiO 2 for thiophene was obviously enhanced, and the adsorption selectivity for thiophene in the presence of aromatics was relatively close to CeO 2 /SiO 2 , attributed to that Ag 2 O/CeO 2 /SiO 2 adsorbed thiophenics via the π-Ag + complexation and S-Ce bonding, where the latter was main interaction. However, there was no synergistic interaction between Ag and Ce species acted as adsorption sites in the Ag 2 O/CeO 2 /SiO 2 , which could be supported by that the chemical state of Ag and Ce in Ag 2 O/CeO 2 /SiO 2 was consistent with corresponding one in Ag 2 O/SiO 2 and CeO 2 /SiO 2 , respectively. Among Ag 2 O/CeO 2 /SiO 2 aerogel composites with different molar ratios of Si/Ce, Ag 2 O/CeO 2 /SiO 2 -50 performed the best, its adsorption uptake for thiophene, benzothiophene and dibenzothiophene from model fuels arrived at 20.4, 21.8 and 27.2 mg-S/g ads , respectively. Langmuir and Freundlich adsorption isotherm models, the pseudo-second-order kinetic model could well describe the adsorption of thiophenics over Ag 2 O/CeO 2 /SiO 2 -50.
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
·
2023
·
IF 6.1
Tong Zhou,Xue Xia,Heping Cui,Yun Zhai,Foxin Zhang,Khizar Hayat,Xiaoming Zhang,Chi-Tang Ho
The influence of pH was studied on volatile flavor formation during thermal treatment of an Amadori rearrangement product (ARP) with or without the addition of cysteine (Cys). The formation of thiols and sulfides or 2-acetylthiazole and pyrazines induced by Cys during thermal degradation of ARP was pH-dependent. At low pH levels, the hydrolysis of Cys to hydrogen sulfide (H2S) was promoted, giving rise to the increase of thiols and sulfides with an obvious meaty aroma. However, alkaline conditions were beneficial for enhancing the cyclization or transformation of imine to the enol structure, which strengthened the formation of 2-acetylthiazole and pyrazines with a roasted and nutty aroma. The imine was derived from the nucleophilic addition of Cys and methylglyoxal (MGO) and subsequent decarboxylation. At pH 8, Cys-induced variation of the flavor profile was weakened during thermal degradation of ARP. Accordingly, the combinational effect of pH and added Cys could be beneficial for achieving the desirable flavors during thermal processing of ARP.
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高影响因子
IONICS
·
2023
·Vol. 29
·期 3
·1019-1028
·
IF 2.8
Zou Yiming,Liu Pufang,Yan Yinglin,Chen Shiyu,Fan Chaojiang,Xu Rongfu,Wang Xianhui,Zhong Lisheng,Yang Rong,Xu Yunhua
Coating conductive polymers on carbon/sulfur (C/S) cathode is an effective strategy for improving electrochemical performances of lithium-sulfur (Li–S) batteries. Furthermore, the heteroatoms in conductive polymer coating exhibit positive effects on electrochemical property. Herein, the C/S cathode was coated by polypyrrole (PPy) and polythiophene (PTh) which were fabricated and systematically investigated to reveal the effect of nitrogen (N) and S heteroatoms on the electrochemical property. As expected, both experimental identification and theoretical calculation verified that the PPy containing N heteroatom-coated C/S cathode possessed strong chemical adsorption capability for soluble polysulfides, which suppressed shuttle effect more effectively and displayed a more stable cycling life, while the PTh@C/S cathode containing S atom presented less Li + diffusion energy barrier, which exhibited reduced polarization and superior rate performance. This work demonstrated the specific functions of N and S heteroatoms in conductive polymer coating on C/S cathode materials, indicating their promising application for advanced Li–S batteries.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Yachun Ren,Yueyang Xu,Erjian Huang,Peng Zhang,Yongping Zeng
Adsorption desulfurization is a very effective method to remove thiophenic compounds from fuels. The metal–organic frameworks (MOFs) have emerged as a new type of desulfurization adsorbents because of their porous nature and large specific surface area. In this study, Cu 2+ was covalently introduced into the UiO-66 framework at the defective sites by the solvothermal method. Further, the π-complexation adsorbent UiO-66-Cu(I) containing Cu + for adsorption desulfurization was synthesized by the methanol vapor-induced reduction. The adsorption performance was tested for the removal of thiophene from the model fuels with different sulfur concentrations. In comparison with the pristine UiO-66, the adsorbent UiO-66-Cu(I) has a higher adsorption capacity for thiophene, reaching 14.8 mg S/g. The competitive adsorption results indicated that UiO-66-Cu(I) has good selectivity for thiophene in the presence of aromatic compounds. From the recycling experiments, this adsorption still has the 86 % of the initial capacity after four cycles, indicating that the adsorbent has a good recycling performance.
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JOURNAL OF RADIOANALYTICAL AND NUCLEAR CHEMISTRY
·
2023
·Vol. 332
·期 10
·4167-4177
·
IF 1.6
Peng Yinyin,Pan Ting,Chen Chuang,Zhou Mi,Liu Derong,Feng Jian,Xiong Wei,Liu Ning,Yuan Guoyuan
In this work, MOFs materials functionalized (HC-MOFs) with heterocyclic ligands (thiophene-TPC, pyrrole-PCA and furfural-FUR) were prepared by a one-step method and used for cobalt ion separation studies. The results showed that the maximum adsorption of cobalt ions by the three adsorbents was 141.0 mg/g (UiO-66-TPC), 146.0 mg/g (UiO-66-PCA), and 150.6 mg/g (UiO-66-FUR), respectively, at pH 8.3 and a temperature of 298 K. In addition, The HC-MOFs showed good stability under different doses (0 ~ 200 kGy) of γ-ray irradiation and have great potential for application in the separation of practical radioactive wastewater containing 60 Co.
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Small
·
2023
·Vol. 19
·期 49
·2304644
·
IF 13.3
Ping Lu,Zhaoyang Qi,Jie Chen,Changshen Ye,Ting Qiu
High-efficiency adsorption of aromatic sulfur-containing compounds from liquid hydrocarbon fuels over metal-organic frameworks (MOFs) is challenging because of inert metal sites. A new method, the Ce-enhanced modulation of MOFs’ microenvironment, is proposed to modulate the –COO···Cu(II)– coordination microenvironment of Hong Kong University of Science and Technology (HKUST-1) using Ce(III) as a molecular scalpel for fabricating abundant high-efficiency Cu(I) and Cu-coordination-unsaturated sites and improving the pore structures around adsorptive sites. The optimal CH-250 thus exhibits adsorptive capacities for 20.2, 28.0, and 58.3 mg S g –1 of thiophene, benzo-thiophene, and dibenzothiophene, respectively, which are superior to most reported MOFs, zeolites, and nanoporous carbons. The constructed Cu(I) sites show stronger affinity for dibenzothiophene (−0.86 eV) than the initial Cu(II) (−0.74 eV) for out-of-plane adsorption. Further, they are far stronger in-plane adsorption interactions in DBT/CH-250 (−0.90 eV) than those in DBT/HKUST-1 (−0.37 eV). Thus, molecular engineering for modulating the coordination microenvironment of MOFs shows great potential for adsorption desulfurization.
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