ChemSusChem
·
2022
·Vol. 15
·期 14
·e202200337
·
IF 9.14
Li-Qi Qiu,Zhi-Wen Yang,Xiangyang Yao,Xiao-Yang Li,Liang-Nian He
Graphical CO 2 photoreduction : Toward building robust artificial photosynthetic systems, a series of single-active-site rhenium bipyridyl complexes with dipyrromethene-BF 2 units exhibit outstanding catalytic efficiency for visible light-driven-CO 2 reduction. New rhenium bipyridyl complexes with dipyrromethene-BF 2 chromophores (A-ReBDP-CZ, A-ReBDP 2 , ReBDP-CZ, and ReBDP 2 ) were developed for highly efficient photocatalytic carbon dioxide (CO 2 ) reduction to carbon monoxide (CO). These catalysts consisted of two moderate electron-deficient groups (dipyrromethene-BF 2 , BDP) as the visible-light-harvesting antenna as well as both electron donor ( N -phenylcarbazole, CZ) and acceptor (BDP) on Re bipyridyl framework. Among ReBDP-CZ and ReBDP 2 complexes, the ReBDP 2 incorporating two electron-deficient BDP chromophores had a longer-lived photoexcited state (182.4 μs) and a twofold enhanced molar absorption coefficient ( ϵ =157000 m −1 cm −1 ) compared with ReBDP-CZ. Thus, ReBDP 2 achieved the superior photocatalytic reactivity and stability with a CO turnover number (TON CO ) value as high as 1323 and quantum yield ( Φ CO ) up to 55 %, which was the most excellent photocatalysis efficiency among the single-active-site Re catalysts without additional photosensitizer. Furthermore, the acetylene-bridged linker was detrimental to the photoactivity and durability of the catalyst. In brief, two BDP-based Re bipyridyl systems with outstanding catalytic performance and significant visible-light-harvesting capabilities in the solar spectrum offer a promising strategy for solar-to-fuel conversion schemes.
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RSC Advances
·
2022
·Vol. 12
·期 13
·8009-8018
·
IF 4.036
Ying Wu,Danying Xing,Linna Zhang,Hualiang Suo,Xiaodan Zhao
Transition metal ion-activated sulfite autoxidation processes for the production of sulfate radicals (SO4˙−) have been widely investigated to achieve efficient abatement of recalcitrant organic pollutants. However, these homogeneous processes suffered from narrow effective pH range and metal release, thus restricting their practical application. In order to address this problem, we report a simple and efficient approach to iohexol abatement by a combined Cu2S and sulfite process (simplified as Cu2S/sulfite process) based on the superior activation performance of copper and the excellent electron donating capacity of the low-valent sulfur species. Compared with typical copper oxides, Cu2S can significantly accelerate the sulfite autoxidation to generate radicals, leading to 100% iohexol abatement in the Cu2S/sulfite process. The influence of solution pH and dissolved oxygen on iohexol abatement is also investigated. Qualitative and quantitative analysis of reactive radicals is performed by electron paramagnetic resonance (EPR) and radical quenching experiments. Generation of SO4˙− from sulfite activation with Cu2S mainly contributes to the iohexol abatement. X-ray photoelectron spectroscopy (XPS) suggests that copper is the main activation site and the reductive sulfur species can achieve the continuous regeneration of copper. Application potential of the Cu2S/sulfite process is also assessed. This study provides a new method for the treatment of water and wastewater containing organic micropollutants.
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JOURNAL OF CHEMICAL THERMODYNAMICS
·
2021
·
IF 3.178
Rongguan Lv,Xuehua Zhang,Rong Xing,Weizhong Shi,Hongkun Zhao,Wanxin Li,Abolghasem Jouyban,William E. Acree
The intermolecular interactions and overall charge distribution of curcumin were respectively investigated by using Hirshfeld surface analysis and molecular electrostatic potential surface. The mole fraction solubility magnitudes of curcumin (I) in aprotic co-solvent blends of DMSO + water, acetone + water and acetonitrile + water ranging from 278.15 to 318.15 (333.15) K under 101.1 kPa was obtained by means of shake-flask method. Under the same conditions, e.g. identical temperature and mass fraction of DMSO (acetone or acetonitrile), the equilibrium solubility of curcumin was greater in DMSO + water blends than in acetone/acetonitrile + water blends. The lowest solubility magnitude was found in neat water at 278.15 K; and the highest one, in acetone/acetonitrile at temperature of T = 318.15 K (aqueous solutions of acetone or acetonitrile) or 333.15 K (aqueous solutions of DMSO). No crystal transition and solvate formation occurred in experimental processes as documented through X-ray power diffraction analysis. The acquired data were correlated by means of the Jouyban-Acree model, Apelblat model and modified van’t Hoff-Jouyban–Acree model. The preferential solvation at 298.15 K was investigated by the approach of inverse Kirkwood–Buff integrals. The parameters of preferential solvation for DMSO, acetone or acetonitrile were positive in the above three blends with middle and DMSO/acetone/acetonitrile-rich composition ranges, which specified that preferential solvation of curcumin was made by co-solvent. The extended Hildebrand solubility approach was further employed to describe the mole fraction solubility at 298.15 K in DMSO/acetone/acetonitrile + water blends studied in the current work and in ethanol/ n -propanol/isopropanol/PG + water blends reported previous by us, obtaining average relative deviations < 5.21%.
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CHEMICAL PHYSICS LETTERS
·
2021
·
IF 2.328
Xi Wang,Jiali Yan,Hao Wang,Daoli Yang,Jinli Zhai,Xiaoya Gao,Chao Gong,Wenjie Zhu,Yongming Luo
To use solar energy effectively, BiOX (Cl, Br, I) nanosheets with reasonable band gap structure were prepared by ultrasonic assisted hydrothermal method. The prepared BiOX (Cl, Br, I) nanosheets removed 90% of CBZ within 5 min, showing rapid degradation kinetic of 0.3858 min −1 . The improved photocatalytic activities can be due to the reduced recombination of photoinduced electron-hole pairs, strong visible-light absorption ability, large surface area and pore. Radicals experiments indicated that the BiOX (Cl, Br, I) generated main holes ( h + ) and minor electrons ( e − ) to degrade CBZ. These results demonstrated the good feasibility of BiOX (Cl, Br, I) nanosheets in the degradation of CBZ under simulated solar light irradiation.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 46
·17281-17289
·
IF 4.39
Dayu Huang,Yue Liu,Qiuyun Ouyang,Hongzhou Lian,Jun Lin
The stability of perovskite quantum dots (PQDs) plays a vital role in practical devices. Besides silica coating, embedding PQDs in zeolites is another strategy to improve their stability significantly. Although the zeolite rigid framework has been reported to protect PQDs, there are few reports on the in situ synthesis of PQDs in zeolites. In this work, cubic phase CsPbX3 (X = Br, I) nanocrystals were successfully prepared by the ion exchange method combined with a non-polar organic trigger. Dropping a certain amount of ZnM2 (M = Br, I) solution into the intermediate product Cs4PbCl6 nanocrystals resulted in the formation of the final CsPbX3 nanocrystals. The ZnM2 solutions were prepared in non-polar solvents (hexane, octane, or chloroform). The highest photoluminescence quantum yield (PLQY) of the synthesized CsPbX3@zeolite composites can reach 83%, with a lifetime of 1.37 μs. The stability of the CsPbX3@zeolite composites thin film against damage from air and light is significantly improved. We fabricated white light-emitting diodes (WLEDs) using CsPbBr3@zeolite as the green light source and CsPbI3@zeolite as the red light source to further emphasize the practical application effect of the CsPbX3@zeolite composites. This work not only provides a new method for the synthesis of CsPbX3 nanocrystals but also involves the in situ synthesis of high stability CsPbX3@zeolite composites within the zeolite.
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Microorganisms
·
2023
·Vol. 12
·期 1
·38
·
IF 4.5
Kun Geng,Ying Lin,Xueyun Zheng,Cheng Li,Shuting Chen,He Ling,Jun Yang,Xiangyu Zhu,Shuli Liang
Acetaldehyde is an important carbonyl compound commonly detected in wines. A high concentration of acetaldehyde can affect the flavor of wines and result in adverse effects on human health. Alcohol dehydrogenase I (ADH1) inSaccharomyces cerevisiaecatalyzes the reduction reaction of acetaldehyde into ethanol in the presence of cofactors, showing the potential to reduce the content of acetaldehyde in wines. In this study,ADH1was successfully expressed inPichia pastorisGS115 based on codon optimization. Then, the expression level ofADH1was enhanced by replacing its promoter with optimized promoters and increasing the copy number of the expression cassette, with ADH1 being purified using nickel column affinity chromatography. The enzymatic activity of purified ADH1 reached 605.44 ± 44.30 U/mg. The results of the effect of ADH1 on the content of acetaldehyde in wine revealed that the acetaldehyde content of wine samples was reduced from 168.05 ± 0.55 to 113.17 ± 6.08 mg/L with the addition of 5 mM NADH and the catalysis of ADH1, and from 135.53 ± 4.08 to 52.89 ± 2.20 mg/L through cofactor regeneration. Our study provides a novel approach to reducing the content of acetaldehyde in wines through enzymatic catalysis.Keywords:alcohol dehydrogenase I;Pichia pastoris;cofactor regeneration;multicopy;acetaldehyde;wine
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Shuai Wang,Anzhe Wang,Pan Gao,Rui Bai,Junjie Liu,Peng Zhou,Dazhao Liu
Strength prediction under the action of pores is crucial for the safety of ceramics. Here, a quantitative prediction model of pore-strength response under mode-I loading was developed based on the new mapping relationship between stress intensity factor and tip radius. The new model was proved to have great application after comparison and analysis of the pore-strength test data of three typical ceramics as well as the pertinent data as-reported in the literature. Results indicated that when the tip radius of pore ( ρ ) exceeds the critical value ( ρ c = K Ic 2 /(π σ 0 2 )), the stress intensity factor increases as a power function with increasing ρ , at which point the strength decay is significantly weakened, and when the ρ is lower than the ρ c , the pore can be equated to a crack problem. This work can not only forecast and assess the failure strength of ceramics containing pores, but also provide guidance for the design of extremely dependable ceramics.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xinman Hu,Fang-Yuan Chen,Jie Ding,Zihe Zhai,Huang Yang,Liyin Shen,Yang Zhu,Dong-Sheng Guo,Changyou Gao
The clinically restored blood supply post myocardial infarction (MI) will break the physiological and metabolic balance of the ischemic myocardial region, leading to a new injury known as myocardial ischemia/reperfusion (I/R) injury. Abundant oxygen brought by the fresh blood would trigger the damaged myocardium to produce excessive reactive oxygen species (ROS) and thereby inflammation along with the recruitment and infiltration of activated neutrophils and macrophages. Inspired by the active targeting process of inflammatory cells, a novel “neutrophil-like” nanoassembly (At@NQA) was prepared by modifying neutrophil membrane fragments onto At@QA NPs containing 1:1 (molar ratio) calixarene molecule (QA) and anti-inflammatory and anti-fibrotic atorvastatin calcium (At). Tail vein injection of the At@NQA could efficiently target the damaged myocardium, inhibit oxidative damage and inflammation, reduce myocardial fibrosis, increase myocardial troponin T (cTnT) and connexin 43 (Cx43) expression, and thus improve cardiac functions effectively.
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Advanced Optical Materials
·
2021
·Vol. 9
·期 8
·2002075
·
IF 9.926
Qin Wang,Mengfeifei Jin,Ya Chen,Yi Zhao,Yao Tong,Ziyao He,Xiaojuan Liang,Weidong Xiang
Currently, high optical purity, perfect stability, and high photoluminescence quantum yield (PLQY) are very important, being the key to obtain high-quality luminescent materials. The research of perovskite nanocrystals (NCs) as optical materials is in full swing. Nevertheless, the low PLQY value, especially for the red-emitting perovskite NCs, is a main obstacle to applications in display. This work reports the optimized components to synthesize CsPb(Br/I) 3 NCs glasses whose PLQY achieves a big boost from 15.4% to ≈ 60% for the first time. Furthermore, the specimens exhibit exceptional tolerance to water and thermal and hence contribute to applicability in high-performance light-emitting diode (LED) and 3D printing. By combining CsPb(Br/I) 3 NCs glass powder and yttrium aluminum garnet (YAG):Ce phosphor with blue chips, the assembled white LEDs reach a high luminous efficiency at 113.0 lm W −1 . The resulting high PLQY is to the benefit of a substantial step toward the practical application of inorganic perovskite materials in the fields of optoelectronic devices and additive manufacturing.
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ELECTROANALYSIS
·
2021
·Vol. 33
·期 7
·1810-1818
·
IF 3.223
Weijia Xu,Tao Liu,Yiqing Wang,Wei Zhang,Xiaoyue Yao,Bailing Hou,Ying Xie,Zhenyu Chu,Wanqin Jin
Cardiac Troponin I (cTnI) is a preferred biomarker to diagnose acute myocardial infarction which is one of the leading risks to health globally due to its short term. However, clinical analyzers are difficult to achieve its on-site quantitative detection. A novel label-free aptasensor was constructed to realize ultrasensitive and rapid recognition of cTnI. A nanocubic AuNPs/In 2 O 3 composite was designed to provide synergistic effects of abundant active sites and signal magnification for aptamers grafting. Relying on a conductance-dependence strategy, this aptasensor can achieve the quantitative detection within 10 min, which is much faster than state-of-the-art analyzers, as well as exhibiting an ultrawide linear range of 0.1–1000 ng/mL and a low detection limit of 0.06 ng/mL with an excellent selectivity in the analysis of human serum.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Weiquan Zhan,Yuan Yuan,Xin Yao,Bingqiao Yang,Feifei Jia,Changsheng Lin,José Luis Arauz-Lara,Shaoxian Song
Developing efficient materials for the extraction of gold(I) was pivotal for application of ammoniacal thiosulfate leaching technology. Mn-doped molybdenum disulfide (Mn-MoS2) spheres were fabricated by a facile hydrothermal route for photocatalytic reduction of the gold(I) thiosulfate complex ([Au(S2O3)2]3–) in this work. The experimental results exhibited that [Au(S2O3)2]3– was efficiently recycled in the form of gold nanoparticles by Mn-MoS2. The reduction capacity (936.9 mg/g) and rate (2.74 mg/(g min) in 300 min) was 1.5 and 2.72 times higher than that of MoS2, respectively. The inside photocatalytic reduction mechanism was studied by combining an experimental and first-principles approach. Outstanding reduction performance of [Au(S2O3)2]3– was attributed to the enhanced transfer of photoinduced electrons after Mn doping. In addition, S atoms in the Mn-S bond could well interact with Au(I), which slightly promoted the adsorption of [Au(S2O3)2]3– on Mn-MoS2. The discovery provided a promising strategy for the efficient extraction of gold(I) from thiosulfate leaching solutions.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 8
·1-9
·
IF 5.833
Leng Yumin,Cheng Jinbing,Liu Congbin,Wang Dong,Lu Zhiwen,Ma Chunhua,Zhang Mengyang,Dong Yuchen,Xing Xiaojing,Yao Lunguang,Chen Zhengbo
A gold nanoparticle (AuNP)–based sensing strategy based on rapid reduction of Au(I→0) is proposed. As a proof-of-concept study, the proposed sensing principle is designed for simultaneous and colorimetric detection and discrimination of multiple proteins. In the presence of H 2 O 2 , the target proteins could reduce Au(I) (i.e. HAuCl 2 ) to AuNPs with different sizes, shapes and dispersion/aggregation states, thus resulting in rapidly colorimetric identification of different proteins. The optical response (i.e. color) of AuNPs is found to be characteristic of a given protein. The color response patterns are characteristic for each protein and can be quantitatively differentiated by statistical techniques. The sensor array is capable of discriminating proteins at concentrations as low as 0.1 μg/mL with high accuracy. A linear relationship was observed between the total Euclidean distances and protein concentration, providing the potential for protein quantification using this sensor array. The limit of detection (LOD) for catalase (Cat) is 0.08 μg/mL. The good linear range (from 0 to 8 μg/mL) has been used for the quantitative assay of Cat. To show a potentially practical application, this method was used to detect and discriminate proteins in human urine and tear samples.
We report a facile gold nanoparticle (AuNP)-based sensing strategy, that is, "a rapid reduction of Au(I) to Au(0) nanoparticles with different sizes and shapes by analytes that having certain reducing capabilities, resulting in different colours." The proposed sensing principle is designed for simultaneous, colorimetric detection and discrimination of multiple proteins.
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