SEPARATION AND PURIFICATION TECHNOLOGY
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2021
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IF 7.312
Yiping Guo,Wei Xie,He Li,Jianping Li,Jun Hu,Honglai Liu
The adsorption desulfurization (ADS) is a promising technology for deep removing thiophene-type sulfurs, yet it remains challenges in maintaining good performance for real applications in the presence of water. Guided by theoretical calculations, we constructed hydrophobic selective channels by crosslinking porous aromatic framework (PAF) of PAF-56 on the surface of adsorbent MOF-199 with Cu nodes reduced. The optimized Cu(I)-BTC@PAF30 shows a high saturated dibenzothiophenes (DBT) adsorption capacity of 61.7 mgS g −1 from the dehydrated model oil. Attributed to the good DBT-affinity (with binding energy (BE) of −90.52 KJ mol −1 ) and water-repulsion (with BE of −14.72 KJ mol −1 ), PAF-56 coating layer significantly improves the hydrophobicity , and keeps the DBT adsorption capacity as high as 50.8 mgS g −1 in the presence of 0.5% (v/v) water, the decline of 17.6% was much smaller than the dramatical 70.9% decrease in pristine Cu(I)-BTC. More importantly, it effectively prevents Cu(I) nodes from the oxidation , and exhibits a superior stable cyclic performance with the removal efficiency above 91% after 20 cycles. Therefore, Cu(I)-BTC@PAF30 can be a good representative of this surface modification strategy to achieve promising application in industrial ADS.
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LWT-FOOD SCIENCE AND TECHNOLOGY
·
2021
·
IF 4.952
Peng Zhang,Chang Chang,Haijie Liu,Qiaojuan Yan,Zhengqiang Jiang
Three protein-rich materials were pretreated with a self-designed alkaline electrolyzed water (AEW) pretreatment equipment to promote the release of angiotensin I-converting enzyme (ACE) inhibitory peptides by improving hydrolysis efficiency. According to degree of hydrolysis (DH) and ACE inhibitory activity, defatted walnut meal (DWM) was selected to study antihypertensive activity by hydrolysis in assistance of AEW pretreatment. It was found DWM pretreated with AEW at pH 11.5 followed by Alcalase hydrolysis exhibited the highest DH (21.96%), protein recovery rate (94.76%), and ACE inhibitory activity (IC 50 of 0.137 mg/mL), in which AEW pretreatment resulted in the transformation of α-helix and β-turn to random coil and the destruction of hydrogen bonds to expose more cleavage sites to enhance hydrolysis efficiency. Thereafter, ACE inhibitory peptides GIENYRVV (IC 50 of 0.102 mg/mL) and AGRISTVNSHTLPVL (IC 50 of 0.20 mg/mL) were identified from the hydrolysate. Overall, AEW pretreatment was an innovative strategy to promote the release of antihypertensive peptides during hydrolysis.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Shixuan Su,Shanshan Li,Jing Hu,Ting Yu,Lingchen Tao,Fuliang Hu,Yunlei Xianyu
Royal jelly as a functional food has great potential to promote human health. As a unique ingredient in royal jelly, 10-hydroxy-2-decenoic acid (10-HDA) is a vital criterion to evaluate the quality of royal jelly. Current approaches for 10-HDA detection mainly rely on high-performance liquid chromatographic (HPLC), but it requires large-scale equipment and skilled technicians that are costly and time-consuming. Herein, we report a colorimetric sensing strategy for 10-HDA detection based on Ag(I) and tetramethylbenzidine (TMB), a widely used chromogenic reagent. Ag(I) can oxidize TMB to generate oxidized TMB (oxTMB) showing a light-blue color. Due to the chelation with Ag (I), the introduction of 10-HDA can prevent the generation of oxTMB that results in a color fading and a decrease in absorbance. This colorimetric sensing strategy enables highly sensitive detection of 10-HDA with a linear range from 1 μM to 10 μM and a limit of detection of 0.13 μM. More importantly, this 10-HDA assay allows for a visual readout either by a smartphone or the naked eye with low cost, convenience, and rapid response that has been successfully applied for evaluating the quality of royal jelly in actual samples. The sensing strategy developed in this work provides a new colorimetric approach that holds great promise as a point-of-care platform for the food industry.
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REACTIVE & FUNCTIONAL POLYMERS
·
2021
·
IF 3.975
Wenchao Zhao,Yanjun Huang,Rong Chen,Hong Peng,Yonggui Liao,Qin Wang
It is a difficult task to remove Ag(I) ions selectively from the complex wastewater containing low concentration of silver(I) ions and high concentration of interfering ions. In this work, the polyhedral oligomeric silsesquioxanes (POSS) hybrid polymer (PSDT) functionalized with thioether/hydroxyl groups was facilely synthesized by photo-initiated thiol-ene polymerization of vinylPOSS and 1, 4-dithiothreitol. The PSDT showed ultrahigh selectivity to Ag(I) ions in a wide pH range, which could completely remove trace level of Ag(I) ions (1 mg L −1 ) from the complex wastewater containing concentrated interfering ions such as Pb(II), Cu(II), Ni(II), Zn(II), Ca(II) and Fe(III) ions (each 200 mg L −1 ), nevertheless, those interfering ions were hardly adsorbed on the PSDT polymer. Moreover, the maximum adsorption capacity for Ag(I) by PSDT was 303 mg g −1 at pH 0.5, and the distribution coefficient ( K d ) for Ag(I) ions could reach 1,620,000 mL g −1 , which was significantly greater than most of the adsorbent materials reported. The high sulfur content (5.93 mmol g −1 ) of nanostructured PSDT and the formation of a stable five-membered Ag(I)-chelated ring may be the major causes for the ultrahigh selective adsorption of Ag(I) ions by PSDT.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Liangzhong Li,Chang Liu,Ruixue Ma,Yunjiang Yu,Zhaofeng Chang,Xiaohui Zhang,Chenyu Yang,Da Chen,Yang Yu,Wei Li,Yongdi Liu
In this study, Fe 3 O 4 @TiO 2 decorated reduced graphene oxide (RGO) nanosheets were synthesized by loading iron oxide on the surface of RGO nanosheets and subsequently coating by titanium oxide, which can be employed as the persulfate (PS) activator and high-performance adsorbent toward thallium (Tl). PS could be effectively activated by the Fe 3 O 4 @TiO 2 decorated RGO nanosheets due to the presence of RGO and Fe(II), resulting in the rapid oxidation of Tl(I) to Tl(III). The removal of Tl(I) was found to be pH-dependent, with the removal efficiency of more than 88.5% in the pH range of 8.0–12.0 at the optimal PS dosage of 10 mM and material dosage of 0.2 g/L. The surface precipitation of Tl 2 O 3 and enhanced adsorption affinity toward Tl were deduced to be main mechanisms for the extremely efficient removal of Tl(I) ions during the oxidation and adsorption hybrid process. The maximum removal capacity of the material at pH 8.0 was estimated as 673.2 mg/g based on the fitting result from the Langmuir model. Approximately 94.7% of ultimate removal capacity could be accomplished within the first 10 min at the initial Tl concentration of 8.5 mg/L. The PS catalytic oxidation coupled with the adsorption technique using the prepared Fe 3 O 4 @TiO 2 decorated RGO nanosheets were proven to be a promising approach for Tl(I) removal from water.
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CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Shuliang Chen,Futing Zi,Xianzhi Hu,Yunlong Chen,Peng Yang,Qiang Wang,Xuecong Qin,Huiling Cheng,Yang Liu,Yi He,Chaowu Wang,Deqiong Hu,Yingmei Liu,Yan Zhang
Silica gel (SG) was modified using 3-mercaptopropyl trimethoxysilane (MPTMS) and used as an adsorbent for the recovery of gold(I) from a thiosulfate solution, based on the hard and soft acids and bases theory. The interfacial properties of the mercaptopropyl-functionalised silica gel (MP–SG) and its performance for the adsorption of gold(I) from a thiosulfate solution were examined. An optimized modification procedure was determined to produce a MP–SG mercapto group content of 1.1 mmol·g −1 . Characterisation of the prepared samples revealed the immobilisation of the MPTMS on the SG surface through chemical adsorption, and that the modification process was accompanied by the release of methanol. The ratio of methanol to the mercapto groups was determined to be 2.06, indicating the formation of 1, 2, or 3 bonds between the SG and MPTMS. The effects of the solution pH, adsorption temperature, thiosulfate concentration and gold concentration on the adsorption of gold(I) onto MP–SG, were also evaluated. The adsorption of gold onto the MP–SG surface was determined to involve ion-interchange between the mercapto groups and Au(S 2 O 3 ) 2 3− . Numerical investigation of the gold adsorption mechanism, revealed that the charge of gold(I) decreased through charge transfer from the ligand to gold(I). The Au–MP–SG could be eluted using mixture of 1% thiourea and 2 mol·L −1 HCl. The findings of this study demonstrate the potential of SG for practical application to gold recovery from a thiosulfate solution.
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OPTICAL MATERIALS
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2019
·
IF 2.687
Jidong Deng,Jiao Xun,Rongxing He
All-inorganic cesium lead halide perovskite nanocrystals (NCs) are promising photoelectric materials for their high photoluminescence quantum yield (PLQY), narrow emission width and tunable optical band gap. Traditionally, the hot injection (HI) method has been utilized to prepare perovskite NCs. However, the HI method requires high temperature, protection under inert gas and other harsh synthetic conditions, which severely hinders large-scale production of these NCs. Herein, we directly synthesized CsPbBr 3 perovskite NCs by a modified LARP (ligand-assisted re-precipitation) approach, and then conducted a specific anion exchange reaction with inexpensive, readily available, non-toxic, and non-polluting KX (X = Cl, I) salts aqueous solution to obtain various compositions of CsPbX 3 perovskite NCs at room temperature (RT). The obtained RT-NCs have high PLQY and outstanding stability, and their photoluminescence can be precisely regulated across the whole visible region (419–670 nm). The use of inorganic salts for the ion exchange provides an efficient method for the design of various halogenated perovskite NCs and their large-scale synthesis at RT.
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ANALYTICAL CHEMISTRY
·
2019
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IF 6.35
Xinfeng Zhang,Xiaoya Fan,Yanying Wang,Fengjie Lei,Lin Li,Juewen Liu,Peng Wu
Aggregation of plasmonic gold nanoparticles (AuNPs) has been widely used for label-free colorimetric sensing. Adding salt is a commonly used method to induce a color change, but salt-induced aggregation by charge screening is a slow kinetic process, making quantitative and reproducible measurement difficult. Herein, we explored an alternative method by charge neutralization using positively charged molecules, such as a DNA-staining dye, SYBR Green I (SG), for efficient and stable assembly of AuNPs. Even submicromolar SG effectively triggered the aggregation of AuNPs in less than 1 min, and the resulting intense blue color was stable for over 10 h. The charge neutralization effect of SG was confirmed with zeta potential measurements. Besides, pH-dependent aggregation of AuNPs by SG agreed well with the pKa of the nitrogen atoms responsible for the positive charges in the SG structure. Moreover, the charge neutralization effect was also observed from polycations such as polyamines. The SG-induced assembly of AuNPs was developed into a label-free colorimetric sensing platform. Benefiting from the intense blue color, this new sensing strategy allowed visual detection of as low as 0.1 nM DNA, 50-fold lower than that by salt. Such a charge neutralization strategy may inspire further thinking on fundamental colloidal science and its applications in analytical chemistry. This work itself significantly improved AuNP-based colorimetric sensors in terms of detection time, signal stability, and sensitivity.
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CATALYSIS LETTERS
·
2019
·Vol. 150
·期 5
·1230-1237
·
IF 2.372
Zeng Rong,Liu Jiachen,Ding Shunmin,Sun Ling,Wu Ling,Cao Lvxin,Qiu Jiaxiang
Abstract Designing catalysts that achieve the rates and selectivities of natural enzymes is a long-standing goal in synthetic chemistry. Herein, the carboxyl-controlled-graphene oxide supported 3-aminopropyl-triethoxysilane (GO n -APTS) heterogeneous catalyts like the class I aldolases with –NH 2 and phenolic –OH groups were developed and applied in aldol reaction. The results demonstrate that the amount of –NH 2 groups and phenolic –OH groups play important roles of activity and selectivity, respectively. The most efficiency catalyst GO 8 -APTS shows an excellent conversion of over 90% with a high aldol product selectivity of about 89%. Furthermore, the catalyst can be easily recovered and reused at least 5 times without significant loss of the reactivity. Graphic Abstract
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2019
·Vol. 26
·期 36
·36776-36785
·
IF 2.914
Ren Zhichang,Wu Wanlin,Yu Ling,Yu Yang
Thallium as a highly toxic metal element has been listed as one of priority drinking water contaminants. In this study, manganese oxide nanoparticles were synthesized through a simple hydrothermal method and applied for the removal of thallium(I). The adsorbent was composed of numerous needle-like nanorods and had an average volume diameter of 230 nm after heat-drying procedure. The crystal form of adsorbent was determined as α -MnO 2 . The adsorbent exhibited a much faster adsorption rate than most of previously reported adsorbent, achieving over 66.4% of equilibrium adsorption capacity in the first 10 min. The adsorption process was found to be highly affected by solution pH and higher than 100 mg/g of adsorption capacity could be obtained in a wide pH range of 6.0–10.0. The isotherm study indicated that the adsorption of Tl(I) on the adsorbent was favorable and governed by a chemisorption process, with the maximum adsorption capacity of 505.5 mg/g at pH 7.0. The adsorption process was confirmed to be thermodynamically spontaneous and endothermic. The presence of Na + , K + , Mg 2+ , Ca 2+ , and Cu 2+ cations had certain negative effects on the uptake of Tl(I). Based on the batch experiments and XPS analysis, the deprotonated hydroxyl groups that bonded to manganese atoms worked as the binding sites for the effective removal of Tl(I) ions and no redox reaction occurred during the adsorption process.
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Qian Ye,Hao Xu,Jing Zhang,Qingguo Wang,Peng Zhou,Yunqi Wang,Xue Huang,Xiaowei Huo,Chaorong Liu,Jinfeng Lu
This work presented a new strategy to activate peroxymonosulfate (PMS) by the addition of nano-zero-valent tungsten (nZVT) via accelerating the redox cycles of Cu(II)/Cu(I), which induce the consecutive generation of highly reactive oxygen species ultimately. The oxidation capacity of the nZVT/Cu(II)/PMS process and the detailed mechanisms of PMS activation were investigated with tetracycline (TC) as the targeted pollutant. Our results indicated that about 70% TC removal was obtained in the nZVT/Cu(II)/PMS system in 15 min with an initial pH of 4.6. In addition, hydroxyl radicals ( OH), sulfate radicals (SO 4 − ), and superoxide radicals ( O 2 − ) were identified as the reactive oxygen species (ROSs) attributed to rapid TC decomposition according to the quenching studies and EPR technology. The effective component that was responsible for PMS activation and ROSs generation was ascertained to be the resulting Cu(I), which derived from the direct reduction pathway driven by epigenetic low valence tungsten species and the indirect reduction pathway driven by active hydrogen atoms. Further, the presence of Cu(II) significantly accelerated the corrosion of the nZVT powders, leading to the accumulation of low valence tungsten species and the decrease in the mean diameter of the ZVT nanoparticles. There was no obvious change of the composition and structure between the original and residual nZVT powders, as evidenced by XPS and XRD analysis. The degradation process of TC included the cleavage of specific functional groups, the ring-opening reactions and the hydroxylation process. This study provided theoretical significance in applying zero-valent metals to activate PMS through a cupric/cuprous redox cycling mechanism.
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ACS Sensors
·
2019
·
IF 6.944
Liping Zhu,Jing Ye,Mengxia Yan,Qiuju Zhu,Shuang Wang,Jianshe Huang,Xiurong Yang
Measurement of cardiac troponin I in the blood is crucial for the early diagnosis of acute myocardial infarction. Herein, a novel and ultrasensitive electrochemiluminescence (ECL) immunosensor has been developed for determination of cardiac troponin I (cTnI) by using Au nanoclusters and hybridization chain reaction (HCR) signal amplification. In this ECL immunosensor, Au nanoclusters were dual-labeled at each end of hairpin DNA (H1 and H2) and acted as the luminophore. DNA initiator strands (T1) and secondary antibody (Ab2) were conjugated on Au nanoparticles (AuNPs) to obtain a smart probe (Ab2-AuNP-T1). In the presence of target cTnI, the sandwiched immunocomplex composed of cTnI, Ab1, and Ab2-AuNP-T1 was formed. Then the initiator strands T1 of Ab2-AuNP-T1 opened the hairpin DNA structures and triggered a cascade of hybridization events. Consequently, a large number of Au NCs were indirectly modified on the surface of the electrode, which could react with the coreactant (K2S2O8) and emit a strong ECL signal. Under the optimal conditions, the immunosensor exhibited a wide detection range for cTnI from 5 fg/mL to 50 ng/mL and a low detection limit of 1.01 fg/mL (S/N = 3). Because of the excellent specificity, stability, and reproducibility of the proposed ECL-HCR sensor, it has a great application prospect for cTnI detection in clinical diagnosis.
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