ACS Applied Energy Materials
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2020
·
IF 4.473
Yiming Wang,Yanchun Yang,Chengjun Zhu,Hongmei Luan,Ruijian Liu,Lei Wang,Chenxi Zhao,Xiaogong Lv
Substitution of Zn with Mg has been reported to suppress CuZn defects, which can improve the photoelectric performance of Cu2ZnSn(S,Se)4 (CZTSSe) photovoltaic devices. In our work, the electrical property enhancement of an absorbing layer can be found by incorporating Mg content into the as-prepared precursor solution, forming an alloyed Cu2MgxZn1-xSn(S,Se)4 (CMZTSSe) phase and increasing the photoelectric performance of devices. By adjusting the doping ratio of Mg, we systemically study the impact of Mg content on the crystal structure, thickness, and electrical properties of the Cu2MgxZn1-xSn(S,Se)4 absorbing layer. Also, the photoelectric performance of Cu2MgxZn1-xSn(S,Se)4 solar cells have a large improvement, and the optimal photoelectric conversion efficiency (PCE) of 7.76% for devices is obtained. Our results offer the finding that Mg doping can optimize the electrical properties of Cu2ZnSn(S,Se)4 photovoltaic devices.
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ACS Omega
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2020
·
IF 2.87
Lu Lu Xiong,Rong Huang,Hui Hui Chai,Ling Yu,Chang Ming Li
A facile, cost-effective, and eco-friendly method was proposed to synthesize Fe3O4@tannic acid@Au nanocomposites (Fe3O4@TA@Au). First, Fe3O4 nanoparticles with diameters of 20 and 200 nm were synthesized by co-precipitation and solvothermal methods, respectively. Gold nanoparticles were deposited on magnetic Fe3O4 through tannic acid-metal-polymer intermediate-layer-mediated reductions. The catalytic activities of the as-prepared Fe3O4@TA@Au were investigated by spectroscopically monitoring the reduction of 4-nitrophenol (4-NP) and methylene blue (MB), which could be achieved within several minutes with an excess of NaBH4. The impact of the Fe3O4 size on the overall catalytic ability of the Fe3O4@TA@Au was systematically studied. The reaction rate constants of the Fe3O4-20 nm@TA@Au for 4-NP and MB reduction were 0.432 and 0.543 min–1, respectively. For the Fe3O4-200 nm@TA@Au nanocomposite, the optimized reaction rate constants for 4-NP and MB reduction were 3.09 and 0.441 min–1, respectively. Due to magnetic separation, the Fe3O4@TA@Au could be easily harvested and recycled. After five recycling cycles, the catalytic ability remained over 90%, and the recycling process could be completed in several minutes, highlighting its potential as a catalyst for 4-NP and MB removal.
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CHEMOSPHERE
·
2020
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IF 5.778
Ping Li,Yixing Wang,Hairong Huang,Shuai Ma,Hu Yang,Zhen-liang Xu
Catalytic membrane plays an important role in environmental remedy. In this study, we reported an Ag coated membrane (PAN-Si-Cu-Ag) with a high catalytic activity to reduce 4-nitrophenol (4-NP) and methyl orange (MO) from water. The best performance is 99% reduction degree and 280 L m −2 .h −1 .bar −1 flux for (4-NP) reduction at 4-NP: NaBH 4 = 1:50 (mM) during a 12-h filtration. The reduction degree for MO is above 90% and the flux is about 230 L m −2 ·h −1 ·bar −1 , which is almost the best report till now. The Ag coated membrane was prepared by metal displacement-epitaxial growth on silica covalent grafted PAN membrane (PAN-Si). Silica atoms were used as linker to ensure the good adhesion between polymer and metal NPs, the loss amount of Ag NPs from the coated catalytic membrane is loss about 2 μg/cm 2 after one month storage. Cheap metal NPs were firstly reduced on the surface of PAN-Si membrane and then used to displace Ag ions. Thus the obtained catalytic membrane showed a very high loading (28%). Finally, the catalytic filtration mechanism of 4-NP was distinguished by Cyclic voltammetry (CV), electrochemical impedance spectroscopy (EIS) and adsorption measurement.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
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2020
·Vol. 413
·期 3
·813-820
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IF 3.637
Dou Nannan,Qu Jianying
In this work, a hybrid of multiwalled carbon nanotubes, nanogold, and reduced graphene (rGO/AuNPs/MWCNTs) was synthesized rapidly with an easy method, and then combined with chitosan (CS), which was fixed on a glassy carbon electrode (GCE) to construct a new kind of electrochemical sensor to simultaneously determine 4-aminophenol (4-AP) and acetaminophen (AC). When detecting 4-AP and AC simultaneously, the linear range is 0.12~12 μM for acetaminophen and 0.05~25 μM for 4-aminophenol; the detection limit is 42 nM for acetaminophen and 2.95 nM for 4-aminophenol. Compared with previously related reports, the proposed sensor has an excellent electrocatalytic performance for the redox of 4-AP and AC, which can effectively determine 4-AP and AC simultaneously in actual samples and has potential application prospect.
Graphical abstract
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CRYSTAL GROWTH & DESIGN
·
2020
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IF 4.089
Taolian Guo,Chao Wang,Nannan Zhang,Yan Zhang,Tian Chen,Xing Xing,Zhenda Lu,Lili Wen
Compared with noble metal nanoparticles (MNPs), non-noble MNPs possess obvious advantages owing to their abundant reserves on the earth and low cost. Therefore, the synthesis of small and highly active non-noble MNPs is desirable in practice. With the merits of metal–organic framework (MOF) nanosheets, we develop a novel and facile in situ reduction strategy for the incorporating of ultrasmall and homogeneous Ni NPs within NMOF-Ni, where the self Ni(II) metal ion nodes are partly reduced to metallic Ni(0) atoms by the reducing agent of aqueous NaBH4 under ambient conditions. The as-synthesized Ni/NMOF-Ni-0.4 behaves as an ideal catalyst for the catalytic reduction of 4-nitrophenol, with high efficiency and selectivity as well as good recyclability, arising from the ultrasmall and monodisperse Ni NPs, as well as 2D MOF nanosheet carriers. Strikingly, the straightforward strategy has been successfully applicable to fabricating Co/NMOF-Co-0.4, illustrating that the in situ reduction method might be facile and effective for producing MNPs/MOFs. This work represents a rare report about fabrication of MNPs/MOFs based on an in situ reduction approach without impregnation of additional metal precursors.
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INTERNATIONAL IMMUNOPHARMACOLOGY
·
2020
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IF 3.943
Dan Li,Jiangping Xu,Yunyun Qin,Ningbo Cai,Yufang Cheng,Haitao Wang
Roflupram (ROF) is a novel phosphodiesterase 4 inhibitor. We previously found that ROF suppressed the production of pro-inflammatory factors in microglial cells; however, the underlying mechanisms are largely unknown. The present study aimed to elucidate the underlying molecular mechanisms of the anti-neuroinflammatory effects of ROF in lipopolysaccharide (LPS)-activated microglial cells and LPS-challenged mice. Treatment with ROF suppressed LPS-induced expression of interleukin (IL)-6 and tumor necrosis factor (TNF)-α in BV-2 microglia cell line. Immunofluorescence and Western blotting analysis showed that ROF significantly inhibited the activation of microglia, as evidenced by decreased expression of ionized calcium binding adaptor molecule-1 (Iba1). Similar results were obtained in primary cultured microglial cells. ROF induced the phosphorylation of AMP-activated protein kinase (AMPK) and the expression of Sirtuin 1 (Sirt1). Interestingly, the AMPK inhibitor, compound C, blocked the role of ROF in both the phosphorylation of AMPK and the expression of Sirt1 in BV-2 cells stimulated with LPS. More importantly, the Sirt1 inhibitor, EX527, abolished the inhibitory role of ROF on the production of pro-inflammatory factors, and reactivated BV-2 cells. In mice challenged with LPS, ROF improved cognition and decreased the levels of IL-6 and TNF-α in both the cortex and hippocampus. In contrast, EX527 weakened the effects of ROF on cognitive enhancement and reduction of pro-inflammatory factors in the cortex and hippocampus. Furthermore, EX527 blocked the inhibitory role of ROF in the activation of microglial cells in both the hippocampus and cortex. Taken together, our results indicated that ROF attenuated LPS-induced neuroinflammatory responses in microglia, and the AMPK/Sirt1 pathway is essential for the anti-inflammatory effects of ROF.
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JOURNAL OF THE CHINESE CHEMICAL SOCIETY
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2020
·Vol. 68
·期 4
·582-591
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IF 1.554
Changzhou Chen,Peng Liu,Haihong Xia,Minghao Zhou,Jianchun Jiang
There is an urgent need to develop a selective hydrogenolysis of C aryl -O bonds in lignin to produce valued-added chemicals and fuels. Recently, hydrogen has been used in the hydrogenation reaction, which hides inevitable danger and is not economical. Therefore, isopropanol, as a hydrogen-donor solvent, is employed for aryl ether hydrogenolysis in lignin models over nickel supported on a carbon nanotube (CNT). Except for aromatic ether (4-O-5), the Ni/CNT catalyst is also found to be suitable for alkyl-aryl ether (α-O-4 and β-O-4) cleavage in control experiments. The physicochemical characterizations were carried out by means of H 2 -temperature-programmed reduction, X-ray diffraction, transmission electron microscopy, and X-ray photoelectron spectroscopy analyses. The catalyst can be magnetically recovered and efficiently reused for five consecutive recycling tests in the transfer hydrogenation of aromatic ethers. A mechanism study indicated that the hydrogenolysis cleavage of the ether bond is the first step in the reaction process, and hydrogenation of aromatic rings is only a successive step in which phenol and benzene are intermediate states and are then further hydrogenated. Furthermore, it has been demonstrated that aryl groups play an important role in the hydrogenation of phenol in the competitive catalytic hydrogenation reaction of phenol.
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Biomedical Materials
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2020
·Vol. 15
·期 4
·045023
·
IF 3.174
Fanchen Sun,Jing Guo,Yuanfa Liu,Yue Yu
In this study, hydrophilic pullulan, which is favorable for cell adhesion, proliferation, and differentiation, was selected as a modifier for the preparation of poly(3-hydroxybutyrate-co-4-hydroxybutyrate) (P(3HB-co-4HB))/pullulan nanofibers via electrospinning to improve the biocompatibility of P(3HB-co-4HB) and increase the drug loading of composite fibers. Alkyl polyglycoside was used as the emulsifying agent to promote emulsification and stabilize the P(3HB-co-4HB)/pullulan composite solution. Drug-loading property of the nanofibers with a shell-core structure is increased because gelatin was not formed into fibers via electrospinning, thereby forming a stable drug-containing gelatin solution in the core layer. Finally, P(3HB-co-4HB)/pullulan-gelatin shell-core nanofibers were prepared. The intermolecular interaction, morphology, crystallization properties, mechanical properties, morphology, sustained release, and biocompatibility of composite nanofibers were characterized. Results show that the crystallization property of P(3HB-co-4HB)/pullulan composite nanofibers increases continuously with an increase in the pullulan content. As the pullulan content increases, the strain and stress of P(3HB-co-4HB)/pullulan nanofibers increase initially and decrease later. At the mass ratio of P(3HB-co-4HB) to pullulan of 10:2, P(3HB-co-4HB)/pullulan composite nanofibers exhibit a uniform morphology with an average diameter of 590 nm and porosity of 70.71%. At this mass ratio, the P(3HB-co-4HB)/pullulan-gelatin/drug shell-core structure, which sustained a release effect for more than 180 h, has potential applications as biomaterials without cytotoxicity.
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MATERIALS CHARACTERIZATION
·
2020
·
IF 3.562
Shuai Ma,Fengjin Xia,Lifeng Dong,Ruibin Jia,Zhenzong Sha,Jie Wang,Yingjie Chen,Beili Pang,Hongzhou Dong,Liyan Yu
Coupling plasmonic gold nanoparticles to sub-stoichiometric copper chalcogenide nanocrystals tends to generate promising nano-heterostructures. We report the research on plasmon-enhanced Cu 2 ZnSn(S 1 − x ,Se x ) 4 -Au nanocomposites (CZTSSe for 0 < x < 1, and CZTS if x = 0), emphasizing on exploring how hetero-epitaxial relationship at Cu 2 ZnSn(S 1 − x ,Se x ) 4 //Au interfaces affects their optoelectronic properties. Digital image processing tools, fast Fourier transform/Fourier inversion, are utilized to extract interfacial epitaxial orientations. We demonstrate that nonnegligible lattice mismatch in short-range order could be equivalently compensated by coincident lattice-matching at certain periodic intervals in a long-range order. By exploring polytypic CZTSSe, we further provide reasonable interpretation of abnormal symmetrical distribution of Au on CZTSSe, which induces lower gold coverage rate and accordingly moderates their localized surface plasmon resonance effect, compared to that of CZTS. It indicates that the shape and phase of CZTSSe should be elaborately controlled to realize optimal multi-site nucleation of heterostructured nanocomposites. As a result, by testing optoelectronic response of solar cells with Cu 2 ZnSn(S 1 − x ,Se x ) 4 -Au films as counter electrodes (CEs), we confirm that a superior hetero-epitaxial interconnection between Au and Cu 2 ZnSn(S 1 − x ,Se x ) 4 can availably restrain interfacial defects of the junction and thus contribute efficient hole transfer/transportation in cathode region. The corresponding balanced electron and hole migration plays a quite significant role in the improvement of open-circuit voltage ( V oc ) and fill factor of photovoltaic devices .
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JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2020
·
IF 4.192
Jingming Wang,Na Zhang,Minyue Zhao,Tingting Jing,Jieyang Jin,Bin Wu,Xiaochun Wan,Wilfried Schwab,Chuankui Song
The carotenoid-derived volatile β-ionone plays an important role in the formation of green and black tea flavors due to its low odor threshold, but its formation and the gene(s) involved in its biosynthesis during the tea withering process is(are) still unknown. In this study, we found that the content of β-ionone increased during the tea withering process catalyzed by an unknown enzyme(s). Correlation analysis of expression patterns of Camellia sinensis carotenoid cleavage dioxygenase genes (CsCCDs) and the β-ionone content during the withering period revealed CsCCD4 as the most promising candidate. The full-length CsCCD4 gene was amplified from C. sinensis, and the biochemical function of the recombinant CsCCD4 protein was studied after coexpression in Escherichia coli strains engineered to accumulate β-carotene. The recombinant protein was able to cleave a variety of carotenoids at the 9–10 and 9′–10′ double bonds. Volatile β-ionone was detected as the main product by gas and liquid chromatography–mass spectrometry. The accumulation of β-ionone was consistent with the expression levels of CsCCD4 in different tissues and during the withering process. The CsCCD4 expression was induced by low temperature and mechanical damage stress but not by dehydration stress. The results demonstrate that CsCCD4 catalyzes the production of β-ionone in the tea plant and provide insight into its formation mechanism during the withering process.
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JOURNAL OF HAZARDOUS MATERIALS
·
2021
·
IF 10.588
Lu Long,Rui Pei,Ya Liu,Xiaoping Rao,Yuanpeng Wang,Shu-feng Zhou,Guowu Zhan
Three-dimensional (3D) printing technology has received remarkable attention in manufacturing catalysts with tailored shapes and high precision, particularly facilitating catalyst recovery, maximizing heat/mass transfer, as well as enhancing catalytic performance. Herein, an engineered recombinant Escherichia coli strain (denoted as e - E. coli ) with overexpressing metallothionein (a metal-binding protein) was explored to synthesize Au nanoparticles serving as both reducing and stabilizing agents. Then, the mixed inks containing e - E. coli /Au composite and biocompatible polymers (sodium alginate and gelatin) were extruded based on a direct ink writing method followed by chemical crosslinking to form robust 3D grids with square symmetry. To boost the mass transfer and minimize pressure drop, the monolith catalysts were assembled into agitating paddles and used for liquid-phase batch reactions (volume: 1 L). As such, the reaction solutions were mixed internally via the powered “catalytic paddles” with high mechanical strength, excellent reactivity, and easy recyclability , which could be reused at least 7 cycles without performance loss. Our work provides a novel strategy for the fabrication of supported Au catalysts, and the proof-of-concept “catalytic paddles” by 3D printing technology can be applied to other industrial solution-based reactions.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Xiangchen Kong,Chao Liu,Ming Lei,Feng Gong,Yue Han,Yuyang Fan,Ming Li,Rui Xiao
The fundamental understanding of the catalytic performance of copper-based catalysts for lignin hydroconversion is delayed compared with the empirical optimization of the catalyst preparation. Herein, we investigate the interplay between the lignin-abundant oxygen-containing functional groups and Cu active species via the catalytic β-O-4 lignin linkage hydrogenolysis. Catalyst performance data and elemental spectra characterizing the catalyst demonstrate the dominance of Cu0 in the catalysis. Remarkably, Cα–OH and Cα═O in the aliphatic chain play critical roles in this process, without which the linkage cannot be broken. These groups markedly accelerate the linkage cleavage by decreasing both the chemisorption energy between Cβ–O and Cu0 and the bond dissociation energy of the linkage. On the contrary, the methoxyl groups attached to the aromatic rings hinder the bond cleavage as a result of the steric effect. Such hindrance is significantly affected by the amount and position of the methoxyl groups. The results of this work highlight the importance of the unique structures of lignin in its reductive depolymerization catalyzed by copper-based catalysts, which appear to offer an opportunity for tailoring efficient copper-based catalysts for lignin hydrogenolysis.
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