JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2022
·
IF 10.319
Long Sun,Lingling Li,Jiajie Fan,Quanlong Xu,Dekun Ma
The rapid charge recombination and low surface reaction kinetics are the two major constraints to the photocatalytic performance of covalent organic frameworks (COFs). To accelerate the charge separation behavior, TpPa-1-COF is decorated with WO 3 via an in-situ growth approach, and the resultant WO 3 /TpPa-1-COF composites show significantly improved photocatalytic performance. Especially, when the WO 3 loading arrives at 3 wt%, 3%WO 3 /TpPa-1-COF exhibits the maximum photocatalytic H 2 evolution rate of 19.89 mmol g −1 h −1 , which is approximately 4.8 times higher than that of pure TpPa-1-COF. The apparent quantum efficiency (AQE) of 3%WO 3 /TpPa-1-COF at 420 nm is detected to be 12.4%. X-ray photoelectron spectroscopy (XPS) characterization confirms the formation of internal electric field between WO 3 and TpPa-1-CF, which can drive the photogenerated charge carrier diffusion in S-scheme mode. As a result, WO 3 /TpPa-1-COF composite possesses high charge separation efficiency and strong redox ability, which is further supported by the photoelectrochemical results, thus benefiting the photocatalysis process. This work provides a rational strategy to modify COFs in photocatalytic water splitting.
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JOURNAL OF ENVIRONMENTAL MANAGEMENT
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2022
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IF 8.91
Lu Wang,Yaqun Yu,Guoqiang Liu,Junhe Lu
Tetrabromobisphenol S (TBBPS), an emerging brominated flame retardant , can cause neurotoxic and cytotoxic effects to human physiology . In this study, the degradation of TBBPS in Co 2+ activated peroxymonosulfate (PMS) oxidation process was explored. In particular, brominated by-products formed during the degradation of the TBBPS were examined. It was found that TBBPS could be effectively removed in the Co 2+ /PMS oxidation process. The pseudo-first-order rate constants were 0.13 min −1 at 0.2 mM PMS and 0.5 μM Co 2+ initially. It appeared that TBBPS degradation occurred via and HO attacks, but played a dominant role. The presence of natural organic matter (NOM) greatly inhibited the transformation of the TBBPS, which can be explained by the scavenging of the radical species. β-Scission, debromination, and cross-coupling were identified as the main reaction pathways of TBBPS degradation in the Co 2+ /PMS system. Further oxidation and ring-opening of the intermediates generated brominated by-products including bromoform, monobromoacetic acid, and dibromoacetic acid. The formation of the brominated by-products increased gradually in approximately 48 h. But, the presence of NOM reduced the yields of the brominated -by-products. The findings of this study indicate that organic bromine contaminants can be effectively removed but lead to brominated by-products in the activated PMS oxidation process, which should be taken into consideration when -based oxidation technology is applied.
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Solar RRL
·
2022
·Vol. 6
·期 8
·2200279
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IF 9.173
Jie Deng,Wanying Lei,Junwei Fu,Huile Jin,Quanlong Xu,Shun Wang
Herein, photocatalytic selective oxidation of hydrocarbons through O 2 represents a promising way for fine chemical industry on account of its mild reaction condition. In this work, Co 3 O 4 -modified BiOBr/AgBr S-scheme heterojunction can effectively oxidize sp 3 C H bonds at benzylic position to its corresponding aldehydes, with a toluene to benzaldehyde selectivity of 94%, which is much higher than that of pure BiOBr (21.7%) and AgBr (58.9%). A unique S-scheme charge-transfer mode is confirmed for the ternary composites by the X-ray photoelectron spectroscopy and reactive species quenching measurement. The remaining photogenerated electrons in AgBr with powerful reduction ability can react with O 2 to generate •O 2 − species, which can further oxidize the benzyl radical formed on the Co 3 O 4 surface to peroxyl radicals and then thermodynamically decompose to benzaldehyde. Herein, this work has important guiding significance for the structure regulation of photocatalysts and application in selective oxidation of sp 3 C H bond of hydrocarbons.
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ACS Applied Nano Materials
·
2022
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IF 6.14
Jingchao Wang,Siyi Li,Kunlong Yang,Tianyong Zhang,Shuang Jiang,Xianggao Li,Bin Li
Coupling heterojunction is an effective and feasible approach to suppressing the electron–hole recombination of a photocatalyst. However, the heterojunction performance is limited by poor interface contact between two semiconductors. Therefore, an in situ partial conversion procedure was proposed to fabricate the flower-spherical BiOI/Bi5O7I (BBOI) heterojunction using bacitracin as a template. The introduction of bacitracin can regulate the assembly of nanosheets into a flower-spherical structure, which caused the BBOI photocatalysts to have larger specific surface areas than BiOI or Bi5O7I. In particular, the dosage of bacitracin can control the thermal conversion of BiOI to Bi5O7I. The in situ partial conversion of BiOI caused the formation of an intimate S-scheme heterojunction interface between BiOI and Bi5O7I, which efficiently inhibited the combination of photogenerated carriers. Upon visible-light irradiation, BBOI-3 exhibited the highest catalytic ability for the simultaneous reduction of Cr(VI) (100%) and oxidative degradation of tetracycline hydrochloride (TH) (80.0%). This work provides an opinion to construct the high-performance heterojunction photocatalysts to environmental remediation.
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MICROCHIMICA ACTA
·
2022
·Vol. 189
·期 5
·1-11
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IF 6.408
Pang Yue-Hong,Wang Yi-Ying,Shen Xiao-Fang,Qiao Jin-Yu
A novel ratiometric electrochemical sensor was developed based on a carbon cloth electrodeposited with silver nanoparticles and drop-coated by covalent organic framework (COF-LZU1) for simultaneous determination of bisphenol A (BPA) and bisphenol S (BPS). Carbon cloth exhibited a significantly larger electrochemical active area than common glassy carbon electrodes (27.5 times). Silver nanoparticles not only provided a stable reference signal but also enhanced electroactivity for the oxidation of BPA and BPS. COF-LZU1 with good adsorption performance and large periodic π-arrays promoted the enrichment of BPA and BPS to further increase the current response. Compared with the traditional single-signal electrochemical sensor, the developed ratiometric sensor exhibited better reproducibility and a wider linear range for BPA and BPS from 0.5 to 100 μ M with a limit of detection of 0.15 μ M. Furthermore, the developed sensor showed excellent stability and superior anti-interference ability. The real sample analysis for BPA and BPS has been successfully carried out in mineral water, electrolyte drink, tea, juice, and beer with recoveries of 88.3–111.7%. The developed ratiometric sensor is expected to be a candidate for the preparation of other electrochemical sensors and the analysis of additional practical samples. Graphical abstract
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高影响因子
HIGH PERFORMANCE POLYMERS
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2022
·
IF 1.73
Yannan Wang,Yajie Wang,Maolian Guo,Tao Ban,Xiuling Zhu
Hydrocarbon-based polymer proton exchange membranes (PEMs) free of heteroatom linkages are supposed to be an attractive alternative for the most advanced perfluorosulfonic acid PEMs, but it is challenging to synthesize them. Here we disclosed a series of aliphatic chain-containing poly(isatin diphenyl-co-terphenyl)(PIDT) copolymers, which were conveniently prepared by superacid-catalyzed Friedel-Crafts polycondensation. Subsequently, the sulfonated copolymer (SPIDT) membranes were prepared by the grafting of side-chain sulfonic acid groups. Due to the formed continuous and efficient nanoscale proton transport channel, these PEMs exhibited excellent proton conductivity showing 186 mS/cm at 80°C, higher than Nafion115 (150 mS/cm). Meanwhile, the prepared membranes exhibited good oxidative stability. The residual weight of the membranes is still greater than 98 wt % after 1 h immersion in Fenton’s reagent at 80°C. Notably, the direct borohydride-hydrogen fuel cell (DBHFC) equipped with SPIDT-50 membrane as the diaphragm showed the peak power density of 71 mW•cm−2 at 25°C, which was greater than that of Nafion115 (63 mW•cm−2). Therefore, the hydrocarbon-based PEMs prepared in this study show promise for application in fuel cells.
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Catalysts
·
2022
·Vol. 12
·期 3
·304
·
IF 4.501
Xinxing Gao,Qianqian Pei,Nianqing Zhu,Yi Mou,Jilei Liang,Xin Zhang,Shoushuai Feng
(S)-N-Boc-3-hydroxypiperidine is an important intermediate of the anticancer drug ibrutinib and is mainly synthesized by the asymmetric reduction catalyzed by ketoreductase coupled with glucose dehydrogenase at present. In this study, the coexpression recombinant strainsE. coli/pET28-K-rbs-G with single promoter andE. coli/pETDuet-K-G with double promoters were first constructed for the coexpression of ketoreductase and glucose dehydrogenase in the same cell. Then, the catalytic efficiency ofE. coli/pET28-K-rbs-G for synthesizing (S)-N-Boc-3-hydroxypiperidine was found to be higher than that ofE. coli/pETDuet-K-G due to the more balanced activity ratio and higher catalytic activity. On this basis, the catalytic conditions ofE. coli/pET28-K-rbs-G were further optimized, and finally both the conversion of the reaction and the optical purity of the product were higher than 99%. In the end, the cell-free extract was proved to be a better catalyst than the whole cell with the improved catalytic efficiency of different recombinant strains. This study developed a better coexpression strategy for ketoreductase and glucose dehydrogenase by investigating the effect of activity ratios and forms of the biocatalysts on the catalytic efficiency deeply, which provided a research basis for the efficient synthesis of chiral compounds.Keywords:(S)-N-Boc-3-hydroxypiperidine;coexpression strategy;activity ratio;ketoreductase;glucose dehydrogenase
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Journal of Physical Chemistry C
·
2022
·
IF 4.177
Yuyao Zhang,Yu Tian,Wen Chen,Min Zhou,Siyong Ou,Yueli Liu
The CO2 photoreduction process is becoming a promising strategy to solve the energy shortage problem and global warming in recent years. How to promote the separation of photoinduced carriers has attracted attention for the improvement of photocatalytic CO2 reduction. In the present work, an S-scheme heterojunction of Bismuthene/CsPbBr3 quantum dots (Bismuthene/CsPbBr3 QDs) is constructed as the photocatalyst for CO2 conversion. As a result, Bismuthene/CsPbBr3 QDs exhibit an optimal CH4 evolution rate of 43.1 μmol h–1 g–1 with 84.53% selectivity over CH4 under ultraviolet–vis light (UV–vis) irradiation. Construction of the S-scheme heterojunction with a narrow band gap semiconductor is the main factor for improving the photocatalytic performance, as the S-scheme heterojunction can suppress the recombination of photoinduced carriers and retain redox ability. The narrow band gap semiconductor Bismuthene can enhance light absorption abilities. This work probably provides some insights for the designing of heterojunction photocatalysts and the improvement of photocatalytic performance.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
·
2023
·
IF 10.9
Tongyu Han,Haifeng Shi,Yigang Chen
Rapid recombination of charge carriers and sluggish Cu 2+ /Cu + conversion rate in Cu-based photocatalysts hinder the improvement of the peroxymonosulfate (PMS) activation efficiency. Herein, a novel S-scheme system was successfully built through hydrothermal and in-situ calcination methods to activate PMS for norfloxacin (NOR) degradation, which combined CuO with BiVO 4 (BVO) containing surface heterojunction. The UV–vis spectra manifested that BVO displayed excellent visible light absorption performance after compounding with CuO, and the light absorption threshold of CuO/BVO was about 600 nm. Thanks to the existence of surface heterojunction in BVO, the photoinduced electrons, and holes would transfer to {010} and {110} facets, respectively. The construction of S-scheme heterojunction further facilitated the accumulation of electrons on CuO, thus realizing the spatial separation of charge carriers. In addition, the electrons gathered on the CuO expedited the Cu 2+ /Cu + cycle, thereby improving the activation efficiency of PMS. On this basis, the NOR removal capacity of 5CuO/BVO composites was obviously enhanced, which was 3.65 and 2.45 times that of CuO and BVO. Moreover, the influence of ambient pH and PMS dosage on the photocatalytic performance of CuO/BVO was investigated. Through the analysis of NOR degradation pathways and degradation products, it was found that the toxicity threat of NOR to the environment was reduced during the degradation process. According to the XPS results, forming the S-scheme heterojunction accelerated the Cu 2+ /Cu + redox cycle during the PMS activating process. Meanwhile, photoluminescence (PL) and time-resolved photoluminescence (TRPL) analysis demonstrated that the CuO/BVO composites exhibited eminent ability for charge separation. The possible mechanism of charge transfer was assumed by exploring reactive species and the energy band structure of catalysts. To sum up, this research provides a new perspective on boosting PMS activation to purify antibiotics in water.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Guanhua Chen,Zhengzheng Wang,Mei Deng,Fangbin Xiao,Xuekun Bai,Hengyi Xu
Foodborne pathogenic microorganism pose a serious threat to public health security; thus, constructing quick and sensitive methods for early screening foodborne pathogenic microorganism is necessary for human health. Teicoplanin (Teic) is a broad-spectrum biometric molecule, which can recognize Gram-positive (G + ) bacteria. In this study, using bovine serum albumin (BSA) and PEG 2k as “carrier” and “linker”, respectively. Teic was wired to magnetic beads (MBs) to form the biomimetic dandelion-like magnetic nanoparticles (MBs-PEG-BSA-Teic) to capture Staphylococcus aureus ( S. aureus ) and Listeria monocytogenes ( L. monocytogenes ). The MBs-PEG-BSA-Teic displayed excellent capture ability of S. aureus (> 93%) and L. monocytogenes (> 86%). After separation, the fluorescence probes were added, forming a “sandwich” structural compounds, namely, MBs-PEG-BSA-Teic~bacteria~fluorescence probes. The fluorescence intensity of the probes was measured by a multimode microplate reader. Consequently, this novel method showed high detection sensitivity to target model bacteria, and the detection limit of S. aureus and L. monocytogenes in PBS buffer solution and juice were achieved 10 1 CFU/mL, spinach and ground beef samples were achieved 10 2 CFU/g. The method has easy operation and high sensitivity, and it is less interfered by food matrix or negative bacteria; thus, this method is suitable for early screening G + pathogen in suspected food samples.
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ACS Applied Energy Materials
·
2021
·
IF 6.024
Tao Long,Bin Xu,Yixin Zhao,Hu Liu,Sheng Cheng,Yongyi Zhang,Jiehua Liu,Fancheng Meng
The shuttling effect and sluggish redox kinetics of polysulfides are the main obstacles that restrict the practical application of lithium–sulfur (Li–S) batteries. Herein, in this work, cathode material embedded with bipolar metals Ti and Co prepared by a facile self-assembly process using hollow carbon nanospheres (HCSs), MXene nanosheets, and CoO(OH) has been reported. Due to the strong chemical adsorption and high catalytic activity introduced by the bipolar metal related active sites, the Li–S battery with the HCS@Co–MXene/S cathode shows the lowest charge transfer resistance and the best rate capability compared with HCS/S and HCS@MXene/S cathodes. Moreover, the battery delivers a high initial discharge capacity of 1309 mA h g–1, which maintains at 570 mA h g–1 after 300 cycles at 0.5 C. Even at an elevated discharge current of 1 C, the battery retains a reversible capacity of 728 mA h g–1 over 120 cycles. Therefore, with the embedding of bipolar metals, the current Li–S battery cathode demonstrates superior cycling stability than the reference cathodes. The findings in this work exhibit a promising prospect for facile assembling of the high-performance Li–S battery cathode and the resultant device.
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Journal of Energy Storage
·
2023
·
IF 9.4
Yangyang Mao,Tianle Li,Siddig Abuelgasim,Xiaoqian Hao,Yupeng Xiao,Chongyang Li,Wenju Wang,Yuqian Li,Encai Bao
Previous studies revealed that LiNO 3 can enhance the cyclic stability of lithium‑sulfur (Li S) batteries by creating a solid electrolyte interface protecting the lithium electrode. However, this study investigated the effect of LiNO 3 and concentration in the electrolyte, first studied under low and high sulfur loading. It is confirmed that adding a small amount of LiNO 3 inhibits the shuttle effect phenomenon in Li S batteries, and the Coulombic efficiency was significantly improved. Appropriately increasing the concentration of LiNO 3 to 2 % could prolong the cycle life. However, when LiNO 3 is excessive, the rate and cycling performance decrease. The design of practical Li S batteries requires more research on the parameters of electrolyte additives under high‑sulfur-loading conditions. After gradient increasing the sulfur loading, the low concentration of LiNO 3 cannot play the best performance of the battery , so it is necessary to improve the concentration of LiNO 3 further. It is evident that adding LiNO 3 in Li S batteries has certain benefits, and the optimal amount of additive is related to the value of sulfur loading.
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