Solar RRL
·
2023
·Vol. 7
·期 17
·2300318
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IF 7.9
Bowen Liu,Xinan Shi,Wei Shao,Jiaxin Gao,Chenxi Zhao,Fuyan Chen,Dongdong Shen,Bingsuo Zou,Daocheng Pan
Cu(In,Ga)(S,Se) 2 (CIGSSe) solar cells are one of the most promising thin film photovoltaics with a record efficiency of 23.6%. However, the biggest drawback to CIGSSe solar cells is their high material cost, partially resulting from relatively rare and expensive indium and gallium. Therefore, improving the utilization of indium and gallium and reducing their wastage can greatly lower the cost of CIGSSe thin film solar cells. Inkjet printing is a facile, cost-effective, and low-waste deposition technology, which is particularly suitable for low-cost and large-area fabrication of CIGSSe solar cells. Herein, a novel and green ionic liquid-assisted ink to fabricate highly efficient CIGSSe solar cells is developed. The material utilization of inkjet printing can be remarkably improved compared to the conventional vacuum-based deposition approach and spin-coating solution approach. The CIGS printable ink is prepared by dissolving copper acetate, indium acetate, gallium nitrate, and thiourea into ethanol with the assistance of n -butylammonium butyrate ionic liquid. Ionic liquid-assisted CIGS ink has a nearly zero wetting angle and a tunable viscosity, which enable to deposit a flat and continuous CIGS thin film by an inkjet printing method. An encouraging power conversion efficiency of 15.22% has been achieved for inkjet-printed CIGSSe solar cells.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
·
IF 9.9
Shuai Li,Ruilin Tang,Chuan Hu,Xiaobin Niu,Liping Wang
As a promising cathode material for high-performance lithium-ion batteries, olivine LiFe 1-x Mn x PO 4 (0 < x < 1, LFMP) combines the high safety of LiFePO 4 and the high energy density of LiMnPO 4 . During the charge-discharge process, poor interface stability of active materials leads to capacity decay, which prevents its commercial application. Here, to stabilize the interface, a new electrolyte additive potassium 2-thienyl tri-fluoroborate (2-TFBP) is developed to boost the performance of LiFe 0.3 Mn 0.7 PO 4 at 4.5 V vs. Li/Li + . Specifically, after 200 cycles, the capacity retention remains at 83.78% in the electrolyte containing 0.2% 2-TFBP while the capacity retention without 2-TFBP addition is only 53.94%. Based on the comprehensive measurements results, the improved cyclic performance is attributed to that 2-TFBP has a higher highest occupied molecular orbit (HOMO) energy and its thiophene group can be electropolymerized above 4.4 V vs. Li/Li + for generating uniform cathode electrolyte interphase (CEI) with poly-thiophene, which can stable materials structure and suppress the decomposition of electrolytes. Meanwhile, 2-TFBP both promotes the deposition/exfoliation of Li + at anode-electrolyte interfaces and regulates Li deposition by K + cations through the electrostatic mechanism. This work presents that 2-TFBP has a great application prospect as a functional additive for high-voltage and high-energy-density lithium metal batteries .
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MATERIALS CHEMISTRY AND PHYSICS
·
2023
·
IF 4.6
Qirun Wang,Yanjie Duan,Zhixiong Huang,Xiaowei Xu,Jichao Shi,Lin Lin,Sheng Han,Runping Jia,Shufang Chang,Dandan Wu
Electrocatalysts with densely exposed sites and high intrinsic activity are desired for high-efficiency oxygen evolution reaction (OER). In this paper, we report the microwave assisted solvothermal growth of NiMoO 4 nanoflowers on electrodeposited Ni(OH) 2 nanosheets , forming a high specific surface area (132.5 m 2 g -1 ) nanoflower-like NiMoO 4 /Ni(OH) 2 configuration supported on a conductive nickel foam (NF) substrate. The as-prepared NiMoO 4 /Ni(OH) 2 /NF behaved efficiently as a self-supported 3D catalyst electrode for alkaline OER, compared with commercial RuO 2 (298 mV overpotential at 10 mA cm −2 and Tafel slope of 88.6 mV dec −1 ), needing a low overpotential of 292 mV to attain 10 mA cm −2 , with a small Tafel slope of 85.0 mV dec −1 and good stability for 100 h running at 10 mA cm −2 in 1.0 M KOH. Aside from enlarged surface area for more exposed edge sites for catalysis, the modulated synergy between Ni and Mo atoms probably contributes to enhanced intrinsic activity. A more electronegative Mo increases the electron density of Ni, thus accelerating the deprotonation of intermediates and driving the transition from Ni to NiOOH, leading to modulated thermodynamics and kinetics for OER catalysis.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-17
·
IF 16.6
Lei Hong,Alu Aqu,Yang Jingyun,He Xi,He Cai,Ren Wenyan,Chen Zimin,Hong Weiqi,Chen Li,He Xuemei,Yang Li,Li Jiong,Wang Zhenling,Wang Wei,Wei Yuquan,Lu Shuaiyao,Lu Guangwen,Song Xiangrong,Wei Xiawei
Mucosal immunity plays a significant role in the first-line defense against viruses transmitted and infected through the respiratory system, such as SARS-CoV-2. However, the lack of effective and safe adjuvants currently limits the development of COVID-19 mucosal vaccines. In the current study, we prepare an intranasal vaccine containing cationic crosslinked carbon dots (CCD) and a SARS-CoV-2 antigen, RBD-HR with spontaneous antigen particlization. Intranasal immunization with CCD/RBD-HR induces high levels of antibodies with broad-spectrum neutralization against authentic viruses/pseudoviruses of Omicron-included variants and protects immunized female BALB/c mice from Omicron infection. Despite strong systemic cellular immune response stimulation, the intranasal CCD/RBD-HR vaccine also induces potent mucosal immunity as determined by the generation of tissue-resident T cells in the lungs and airway. Moreover, CCD/RBD-HR not only activates professional antigen-presenting cells (APCs), dendritic cells, but also effectively targets nasal epithelial cells, promotes antigen binding via sialic acid, and surprisingly provokes the antigen-presenting of nasal epithelial cells. We demonstrate that CCD is a promising intranasal vaccine adjuvant for provoking strong mucosal immunity and might be a candidate adjuvant for intranasal vaccine development for many types of infectious diseases, including COVID-19.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Xianping Deng,Peiwen Wu,Xiaodong Du,Guining Lu,Yanyan Gong,Zhi Dang,Dongye Zhao
Combined heavy metals and chlorinated organic compounds have been widely reported in industrial wastewater. Yet, simultaneous removal of these contaminants remains challenging. In this study, a bi-functional composite (TNTs@AC) was prepared based on commercial titanium dioxide (TiO 2 ) and activated carbon (AC) and tested for simultaneous removal of Cd(II) and 2-chlorophenol (2-CP). Under the action of high temperature and pressure, TiO 2 was transformed into titanate nanotubes (TNTs) and bound to AC, and in the meanwhile, nanoscale AC particles were patched on the TNTs. In the mixed TNTs and AC phases, TNTs was responsible for taking up Cd(II), whereas AC for 2-CP. As such, the relative adsorption capacities of the composite for Cd(II) and 2-CP varied with the mass ratio of TiO 2 :AC, with decent uptakes for both chemicals in the mass ratio rage of 1:3 ∼1:1. TNTs@AC (prepared at TiO 2 :AC = 1:1) demonstrated fast sorption kinetics and high sorption capacities for both Cd(II) and 2-CP, with a maximum Langmuir adsorption capacity of 109 and 52 mg/g, respectively, in the single solute systems. In the binary systems, the adsorption capacity of Cd(II) was not affected by the presence of 2-CP, whereas the presence of Cd(II) slightly increased the uptake of 2-CP in the low Cd concentration domain (final Cd < 7 mg/L) but mildly inhibited the uptake at Cd > 7 mg/L. The dominant adsorption mechanism of Cd(II) was ion exchange between Cd(II) and Na + /H + of the -ONa/H group of TNTs; while AC served as the primary sink for 2-CP via hydrophobic interaction along with some other possible mechanisms such as surface complexation and hole filling. TNTs@AC also performed well under common environmental conditions (pH, common co-ions, and dissolved organic matter). The formation of mixed TNTs and AC microphases appears promising for simultaneous removal of heavy metals and organic compounds from contaminated water.
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ACS Catalysis
·
2023
·
IF 12.9
Zhe-Ming Wu,Feng Xie,Wen Zheng,Chang-Feng Liu,Chao-Ping Lin,Ren-Chao Zheng,Yu-Guo Zheng
Amidases are robust biocatalysts for the industrial synthesis of carboxylic acids. Amidase-catalyzed hydrolysis of 2-chloronicotinamide is regarded as a promising route for 2-chloronicotinic acid production, which is an important building block for agrochemicals and pharmaceuticals. However, the o-substituted Cl of the pyridine ring caused a strong electronic effect and steric hindrance. Engineering access tunnels is one of the most efficient strategies to improve catalytic efficiency by adjusting the transfer efficiency of ligands. Herein, we engineered a twisted access tunnel of amidase and the mutant PaAmiM1A378V+V402L+L403V was achieved, which exhibited increased catalytic efficiency toward 2-chloronicotinamide. Tunnel analysis, molecular dynamics simulations, and quantum mechanical calculations revealed that the straightened tunnel significantly improved the transport efficiency and simultaneously facilitated substrate binding and nucleophilic attack. With the best mutant as a biocatalyst, 1330 mM product was accumulated within 2 h and a high space-time-yield of 2515 gproduct L–1 d–1 was achieved, which is the highest ever reported. These results lay the foundation for industrial production of 2-chloronicotinic acid and give important guidance for engineering amidases into versatile biocatalysts.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Lu-Qing Xie,Sui Peng,Ya-Nan Xin,Bo Liu,Xin-Yu Jiang,Jin-Gang Yu
A novel 3-dimensional graphene oxide/2-mercaptothiazoline (3D GO-MT) aerogel was prepared by using GO and MT which contains heteroatoms (nitrogen-, sulfur-) through a facile hydrothermal assembly process and a following freeze-drying technology . The effects of hydrothermal reaction temperature and GO-to-MT mass ratio on the physicochemical properties of the composites were investigated. The removal of Cu 2+ from aqueous solution by 3D GO-MT aerogels was evaluated. The results showed that the composite (GO-MT 1:3/100 °C ) with GO-to-MT mass ratio of 1:3 prepared at 100 °C had the highest adsorption capacity for Cu 2+ (0.5299 mmol g −1 ). In a bicomponent system of Cu 2+ /Pb 2+ , GO-MT 1:3/100 °C exhibited higher adsorption selectivity for Cu 2+ . And the distribution coefficients K of GO-MT 1:3/100 ° C for Cu 2+ /Y 3+ , Cu 2+ /Nd 3+ in the bicomponent systems were 0.6224 and 0.1253, respectively. The morphology and composition of GO-MT 1:3/100 °C , as well as the adsorption mechanism for Cu 2+ were investigated by scanning electron microscopy, Brunauer-Emmett-Teller, elemental analysis, Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy. The presence of nitrogen and sulfur on MT heterocycle promoted the possible assembly of MT with GO through π-π stacking and hydrogen bonding interactions. Additionally, the existence of these heteroatoms in MT dominated the metal-chelate affinity of 3D GO-MT aerogel for selective adsorption of Cu 2+ . The fitted data of kinetics and thermodynamics showed that the adsorption process followed linear pseudo-second-order kinetics and linear Langmuir isotherm model. The adsorption process is non spontaneous and endothermic. The adsorption mechanism of GO-MT 1:3/100 °C for Cu 2+ involves coordination, cation-π electron interaction, electrostatic attraction and other intermolecular interactions. 3D GO-MT 1:3/100 °C can be used as an adsorbent material for selective adsorption/enrichment of Cu 2+ in aqueous solution.
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Molecular Catalysis
·
2023
·
IF 4.6
Tongyun Zhang,Chengping Zhang,Xiaoxun Ma,Hengdao Quan
3,3,3-trifluoropropyne (HFY-2223tz) is a novel refrigerant with great physicochemical properties. Though preparation of HFY-2223tz from halogenated olefins is theoretically effective, it remains great challenges for dehydrohalogenation from halogenated olefins, limiting the detailed knowledge. Here, we established a facile investigation to explore the gas-phase dehydrochlorination reaction of 2‑chloro-3,3,3-trifluoropropene (HCFO-1233xf) over various halides (Na, K, Rb, Cs) supported active carbon (AC) catalysts. The CsF was concluded as the optimal active component with best dehydrochlorination selectivity and conversion of HCFO-1233xf. The CO 2 -TPD results illustrated that dehydrochlorination of HCFO-1233xf proceeded through E1cB mechanism. Mechanism study revealed the evolution of side-products including ( Z / E )-1,3,3,3-tetrafluoropropylene, 2,3,3,3-tetrafluoropropylene, ( Z / E )-1‑chloro‑3,3,3-trifluoroproene, and 3,3,3-trifluoroprop-1-ene, etc. However, observable deactivation of CsF catalyst was noticed, which, according to combined XRD and XPS results and density functional theory (DFT) calculations, was attributed to the F/Cl exchange between HCFO-1233xf and catalyst, leading to rapid fluorine consumption. This work thus provides basic knowledge about heterogeneous catalytic synthesis of HFY-2223tz from dehydrohalogenation of halogenated olefins.
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DALTON TRANSACTIONS
·
2023
·
IF 4
Yuanlei Huang,Mengdi Lv,Binglian Guo,Guojing Hu,Yong Qian,Zhi Su,Xuling Xue,Hong-Ke Liu
Breast cancer (BC) is one of the most common malignant tumors and often accompanied by inflammatory processes. Inflammation is an essential component of the tumor microenvironment, which might influence tumor proliferation and metastasis. Herein, three metal–arene complexes MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru were prepared by tethering the non-steroidal anti-inflammatory drug meclofenamic acid (MA). Among them, MA-bip-Ru and MA-bpy-Ir showed lower cytotoxicity towards cancer cells, but MA-bpy-Ru showed significantly high selectivity and cytotoxicity towards MCF-7 cells through the autophagic pathway and exhibited no toxicity against normal HLF cells, showing potential for selective treatment of tumor cells. MA-bpy-Ru could also effectively destroy the 3D multicellular tumor spheroids, demonstrating its potential for clinical application. Besides, MA-bip-Ru, MA-bpy-Ir, and MA-bpy-Ru exhibited anti-inflammatory properties superior to MA, notably downregulating the expression of cyclooxygenase-2 (COX-2) and inhibiting the secretion of prostaglandin E2 in vitro. These findings demonstrated that MA-bpy-Ru was capable of intervening in inflammatory processes and showed the potential of MA-bpy-Ru to act as a selective anticancer agent, thus presenting a new mechanism of action for metal–arene complexes.
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CHEMOSPHERE
·
2023
·
IF 8.8
Xuan Zhang,Keke Geng,Ningning Wu,Gang Hu,Ben Fan,Jian He,Wenjing Qiao
4-Chloro-2-methylphenoxyacetic acid (MCPA) is a widely used herbicide across the world. MCPA is persistent and easily transports into anoxic environment, such as groundwater, sediments and deep soils. However, little research on anaerobic microbial degradation of MCPA was carried out. The functional microorganisms as well as the catabolic pathway are still unknown. In this research, an anaerobic MCPA-degrading bacterial consortium was enriched from the river sediment near a pesticide-manufacturing plant. After about 6 months’ acclimation , the MCPA transformation rate of the consortium reached 4.32 μmol g −1 day −1 , 25 times faster than that of the original sludge . 96% of added MCPA (2.5 mM) was degraded within 9 d of incubation. Three metabolites including 4-chloro-2-methylphenol (MCP), 2-methylphenol (2-MP) and phenol were identified during the anaerobic degradation of MCPA. An anaerobic catabolic pathway was firstly proposed: firstly, MCPA was transformed to MCP via the cleavage of the aryl ether, then MCP was reductively dechlorinated to 2-MP which was further demethylated to phenol. The 16S rRNA gene amplicon sequencing revealed a substantial shift in the bacterial community composition after the acclimation. SBR1031, Acidaminococcaceae , Aminicenantales , Syntrophorhabdus , Acidaminobacter , Bacteroidetes_vadinHA17 , Methanosaeta , Bathyarchaeia , KD4-96, Anaeromyxobacter , and Dehalobacter were significantly increased in the enriched consortium after acclimation, and positively correlated with the anaerobic degradation of MCPA as suggested by heat map correlation analysis. This study provides a basis for further elucidation of the anaerobic catabolism of MCPA, and contributes to developing efficient and low-cost anaerobic treatment technologies for MCPA pollution.
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Inorganic Chemistry Frontiers
·
2023
·Vol. 10
·期 7
·2107-2114
·
IF 7
Qin Wang,Jinxuan Ren,Dan Wang,Liling Cao,Xuehua Dong,Ling Huang,Daojiang Gao,Guohong Zou
Two fluorine antimony nitrates named (NH4)3SbF3(NO3)3 and (NH4)3SbF4(NO3)2 have been successfully synthesized by a low temperature molten salt method. Although these two title compounds possess NO3− groups and similar Sb-polyhedra, they exhibit completely different macroscopic centricities, (NH4)3SbF3(NO3)3 being noncentrosymmetric while (NH4)3SbF4(NO3)2 being centrosymmetric, which is induced by the discrepant coordination environments of Sb3+. Interestingly, the noncentrosymmetric (NH4)3SbF3(NO3)3 exhibits a strong second harmonic generation response (3.3 × KDP), a large birefringence (0.098@546 nm) and a large band gap (3.77 eV), indicating its potential as a UV nonlinear optical material. Detailed structure–property analysis confirms that the superior optical property is due to the synergistic effect of the planar π-conjugated NO3− groups and the stereochemically active lone pair containing Sb3+ cations.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2023
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IF 9.8
Xiaolong Yu,Huanhuan Xing,Jianteng Sun,Xiaodong Du,Guining Lu,Lizhong Zhu
Di-(2-ethylhexyl) phthalate (DEHP) as widely utilized plasticizer has aroused increasing concerns since its endocrine disrupting effects and continuous accumulation in biota. To date, the interaction mechanism between DEHP and rice plants has not been clearly illustrated at molecular level. Here, we investigated biological transformation and response of rice plants ( Oryza sativa L.) to DEHP at realistic exposure concentrations. Nontargeted screening by UPLC-QTOF-MS was used to verify 21 transformation products derived from phase I metabolism (hydroxylation and hydrolysis) and phase II metabolism (conjugation with amino acids, glutathione, and carbohydrates) in rice. MEHHP-asp, MEHHP-tyr, MEHHP-ala, MECPP-tyr and MEOHP-tyr as the conjugation products with amino acids are observed for the first time. Transcriptomics analyses unraveled that DEHP exposure had strong negative effects on genes associated with antioxidative components synthesis, DNA binding, nucleotide excision repair, intracellular homeostasis, and anabolism. Untargeted metabolomics revealed that metabolic network reprogramming in rice roots was induced by DEHP, including nucleotide metabolism, carbohydrate metabolism, amino acid synthesis, lipid metabolism, synthesis of antioxidant component, organic acid metabolism and phenylpropanoid biosynthesis. The integrated analyses of interaction between differentially expressed genes (DEGs) and differentially expressed metabolites (DEMs) endorsed that metabolic network regulated by DEGs was significantly interfered by DEHP, resulting in cell dysfunction of roots and visible growth inhibition. Overall, these finding generated fresh perspective for crops security caused by plasticizer pollution and enhanced the public focus on dietary risk.
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危险品化学品经营许可证（带存储）