MICROCHIMICA ACTA
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2023
·Vol. 190
·期 8
·1-8
·
IF 5.7
Xu Feifei,Li Xinyang,Chen Chen,Liang Zhigang,Xu Guanhong,Wei Fangdi,Yang Jing,Hu Qin,Cen Yao
A fast, eco-friendly and accurate ratiometric fluorescent strategy is presented for the determination of organophosphorus pesticides (OPs) using intrinsic dual-emission silica nanoparticles modified with Rhodamine 6G (SiNPs-Rho6G). SiNPs-Rho6G had intrinsic dual-emission at 410 and 550 nm. The substrate acetylcholine was catalyzed by acetylcholinesterase (AChE) to produce thiocholine (TCh). TCh triggered the specific reaction of Ellman's reagent 5, 5-dithiobis (2-nitrobenzoic acid) to obtain 5-thio-2-nitrobenzoic acid, which caused the decrease in fluorescence intensity of SiNPs-Rho6G at 410 nm by the inner filter effect, while the fluorescence intensity of SiNPs-Rho6G at 550 nm was not significantly changed. OPs caused the recovery of the fluorescence at 410 nm by inhibiting the activity of AChE. Thus, the quantitative detection of OPs could be achieved through utilizing the catalytic characteristic of AChE. The linear curve from 0.010 to 0.250 μg mL -1 with a detection limit of 7 ng mL -1 was obtained for the determination of chlorpyrifos (Cpf). The ratiometric probe was used to detect the spiked Cpf in environmental and food samples with good recoveries. Therefore, combined with the dual emission characteristics of SiNPs-Rho6G and the specificity of the enzyme, the ratio fluorescence sensing platform has potential application prospects in OPs determinations. Graphical Abstract
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Nano Research
·
2023
·
IF 9.9
Wang Yaya,Wen Yunzhou,Cheng Yumeng,Chen Xinhong,Zhuansun Mengjiao,Wang Tongbao,Li Jun,Meira Debora,Sun Huarui,Wei Jun,Zhou Jia,Wang Yuhang,He Sisi
The polymer electrolyte membrane (PEM) electrolyzers are burdened with costly iridium (Ir)-based catalysts and high operation overpotentials for the oxygen evolution reaction (OER). The development of earth-abundant, highly active, and durable electrocatalysts to replace Ir is a critical step in reducing the cost of green hydrogen production. Here we develop a Ru 5 Mo 4 O x binary oxide catalyst that exhibits high activity and stability in acidic OER. The electron-withdrawing property of Mo enriches the electrophilic surface oxygen species, which promotes acidic OER to proceed via the adsorbate evolution pathway. As a result, we achieve a 189 mV overpotential at 10 mA·cm −2 and a Tafel slope of 48.8 mV·dec −1 . Our catalyst demonstrates a substantial 18-fold increase in intrinsic activity, as evaluated by turnover frequency, compared to commercially available RuO 2 and IrO 2 catalysts. Moreover, we report a stable OER operation at 10 mA·cm −2 for 100 h with a low degradation rate of 2.05 mV·h −1 .
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-10
·
IF 16.6
Du Jiannan,Han Guokang,Zhang Wei,Li Lingfeng,Yan Yuqi,Shi Yaoxuan,Zhang Xue,Geng Lin,Wang Zhijiang,Xiong Yueping,Yin Geping,Du Chunyu
The two-electron oxygen reduction reaction in acid is highly attractive to produce H 2 O 2 , a commodity chemical vital in various industry and household scenarios, which is still hindered by the sluggish reaction kinetics. Herein, both density function theory calculation and in-situ characterization demonstrate that in dual-atom CoIn catalyst, O-affinitive In atom triggers the favorable and stable adsorption of hydroxyl, which effectively optimizes the adsorption of OOH on neighboring Co. As a result, the oxygen reduction on Co atoms shifts to two-electron pathway for efficient H 2 O 2 production in acid. The H 2 O 2 partial current density reaches 1.92 mA cm −2 at 0.65 V in the rotating ring-disk electrode test, while the H 2 O 2 production rate is as high as 9.68 mol g −1 h −1 in the three-phase flow cell. Additionally, the CoIn-N-C presents excellent stability during the long-term operation, verifying the practicability of the CoIn-N-C catalyst. This work provides inspiring insights into the rational design of active catalysts for H 2 O 2 production and other catalytic systems.
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JOURNAL OF SOLID STATE ELECTROCHEMISTRY
·
2023
·
IF 2.5
Liu Wenjun,Guan Jinyu,Kong Bo,Lu Hongbing,Wu Yu,Qin XiaoLi,Jiang Hongmei,Liu Xiaoying
The severe toxicity of heavy metal ions (HMIs) to both the environment safety and human health makes it challenging to build a system that can simultaneously detect them. A method simultaneous electrochemical detection of Cd 2+ and Pb 2+ was developed here using amino-functionalized bismuth-based metal–organic frameworks (NH 2 -Bi-MOFs) and graphene aerogels (GAs) composites. The GAs/NH 2 -Bi-MOFs composites were made by ultrasonically depositing the NH 2 -Bi-MOF on the GAs. GAs support NH 2 -Bi-MOFs and boost their conductivity by accelerating electron transmission through the matrix. NH 2 -Bi-MOFs acted as a binding site for Cd 2+ and Pb 2+ , because hydrophilic groups (-NH 2 ) and bismuth metal active sites collaborated. The GAs/NH 2 -Bi-MOFs composite–modified electrodes detection capability was assessed. The proposed electrochemical sensor can be effectively used for individual and simultaneous detection of the Cd 2+ and Pb 2+ in aqueous solutions with outstanding sensitivity and interference used to simultaneously detect Cd 2+ and Pb 2+ in river water and tap water samples with satisfactory accuracy and repeatability. This paper provides a unique technique for concurrently detecting Cd 2+ and Pb 2+ in practical applications.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Zhu Guo-Rui,Zhang Qin,Liu Qing-Song,Bai Qi-Yao,Quan Yi-Zhou,Gao You,Wu Gang,Wang Yu-Zhong
As a replacement for highly flammable and volatile organic liquid electrolyte, solid polymer electrolyte shows attractive practical prospect in high-energy lithium metal batteries. However, unsatisfied interface performance and ionic conductivities are two critical challenges. A common strategy involves introducing organic solvents or plasticizers, but this violates the original intention of security design. Here, an electrolyte concept called liquid polymer electrolyte without any small molecular solvents is proposed for safe and high-performance batteries, based on the design of a room-temperature liquid-state brush-like polymer as the sole solvent of lithium salts. This liquid polymer electrolyte is non-flammable and exhibits high ionic conductivity (1.09 \(\times\) 10 −4 S cm −1 at 25 °C), significant lithium dendrite suppression, and stable long-term cycling over a wide operating temperature range ( ≥ 1000 cycles at 60 °C and 90 °C). Moreover, the pouch cell can resist thermal abuse, vacuum environment, and mechanical abuse. This electrolyte and design strategy are expected to provide enlightening ideas for the development of safe and high-performance polymer electrolytes.
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MOLECULAR NEUROBIOLOGY
·
2023
·
IF 5.1
Hua Wei,Ma Shuainan,Pang Yuxin,Liu Qi,Wang Yueying,Liu Zhiyi,Zhao Nan,Ren Naixin,Jin Sinan,Wang Benshuai,Song Yuejia,Qi Jiping
Intracerebral hemorrhage (ICH) is a lethal stroke with high mortality or disability. However, effective therapy for ICH damage is generally lacking. Previous investigations have suggested that lysosomal protein transmembrane 5 (LAPTM5) is involved in various pathological processes, including autophagy, apoptosis, and inflammation. In this study, we aimed to identify the expression and functions of LAPTM5 in collagenase-induced ICH mouse models and hemoglobin-induced cell models. We found that LAPTM5 was highly expressed in brain tissues around the hematoma, and double immunostaining studies showed that LAPTM5 was co-expressed with microglia cells, neurons, and astrocytes. Following ICH, the mice presented increased brain edema, blood-brain barrier permeability, and neurological deficits, while pathological symptoms were alleviated after the LAPTM5 knockdown. Adeno-associated virus 9-mediated downregulation of LAPTM5 also improves ICH-induced secondary cerebral damage, including neuronal degeneration, the polarization of M1-like microglia, and inflammatory cascades. Furthermore, LAPTM5 promoted activation of the nuclear factor kappa-B (NF-κB) pathway in response to neuroinflammation. Further investigations indicated that brain injury improved by LAPTM5 knockdown was further exacerbated after the overexpression of receptor-interacting protein kinase 1 ( RIP1 ), which is revealed to trigger the NF-κB pathway. In vitro experiments demonstrated that LAPTM5 silencing inhibited hemoglobin-induced cell function and confirmed regulation between RIP1 and LAPTM5. In conclusion, the present study indicates that LAPTM5 may act as a positive regulator in the context of ICH by modulating the RIP1/NF-κB pathway. Thus, it may be a candidate gene for further study of molecular or therapeutic targets.
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MOLECULAR MEDICINE
·
2023
·Vol. 29
·期 1
·1-19
·
IF 5.7
Han Zhiyang,Hu Haidi,Yin MingZhu,Lin Yu,Yan Yan,Han Peng,Liu Bing,Jing Bao
Background Macrophage-like transformation of vascular smooth muscle cells (VSMCs) is a risk factor of atherosclerosis (AS) progression. Transcription factor homeobox A1 (HOXA1) plays functional roles in differentiation and development. This study aims to explore the role of HOXA1 in VSMC transformation, thereby providing evidence for the potential mechanism of AS pathogenesis.Methods High fat diet (HFD)-fed apolipoprotein E knockout (ApoE−/−) mice were applied as an in vivo model to imitate AS, while 1-palmitoyl-2-(5-oxovaleroyl)-sn-glycero-3-phosphocholine (POV-PC)-treated VSMCs were applied as an in vitro model. Recombinant adeno-associated-virus-1 (AAV-1) vectors that express short-hairpin RNAs targeting HOXA1, herein referred as AAV1-shHOXA1, were generated for the loss-of-function experiments throughout the study.Results In the aortic root of AS mice, lipid deposition was severer and HOXA1 expression was higher than the wide-type mice fed with normal diet or HFD. Silencing of HOXA1 inhibited the AS-induced weight gain, inflammatory response, serum and liver lipid metabolism disorder and atherosclerotic plaque formation. Besides, lesions from AS mice with HOXA1 knockdown showed less trans-differentiation of VSMCs to macrophage-like cells, along with a suppression of krüppel-like factor 4 (KLF4) and nuclear factor (NF)-κB RelA (p65) expression. In vitro experiments consistently confirmed that HOXA1 knockdown suppressed lipid accumulation, VSMC-to-macrophage phenotypic switch and inflammation in POV-PC-treated VSMCs. Mechanism investigations further illustrated that HOXA1 transcriptionally activated RelA and KLF4 to participate in the pathological manifestations of VSMCs.Conclusion sHOXA1 participates in AS progression by regulating VSMCs plasticity via regulation of NF-κB p65 and KLF4. HOXA1 has the potential to be a biomarker or therapeutic target for AS.
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POLYMER BULLETIN
·
2023
·
IF 3.2
Song Jie,Han Jiaxuan,Zhang Rong,Dou Yufang,Li Shenggang,Zhang Min
This study extracted an antibacterial component from the natural plant Plantago asiatica L. to gain Plantago extract (PTE); PTE was then compounded with polybutylene succinate (PBS) to prepare an antibacterial composite material. To further improve the compatibility of PBS and PTE, chitosan (CS) and hydroxypropyl- β -cyclodextrin (H- β -CD) were used to modify PTE, resulting in the preparation of CS-PTE microcapsules and (H- β -CD)-PTE microcapsules. And CS-PTE microcapsules and (H- β -CD)-PTE microcapsules were added to PBS at different ratios to prepare PBS/CS-PTE and PBS/(H- β -CD)-PTE composite materials. FTIR and SEM tests showed that both microcapsules were successfully prepared and confirmed the antibacterial activity of PTE by inhibition circles method. The binding energy of the composites shifted slightly, indicating that the microcapsules formed intermolecular forces with PBS. The 2 θ angular strength of XRD gradually weakened with the increase in microcapsule addition, and the crystallinity decreased, as well as the thermal and mechanical properties. However, the thermal properties were better than those of PTE/PBS composites, and the thermal properties better than PTE/PBS composites. The hydrophilicity of PBS/(H- β -CD)-PTE composites improved significantly with the addition of microcapsules. The molecular simulation results showed that the intermolecular interaction between PBS and CS-lignans was stronger, and its compatibility was better.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 41
·94195-94204
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IF 5.8
Zhao Dandan,Fu Chen,Lin Sudan,Xu Yongzhi,He Haoran,Liu Siyuan,Shi Xueqing
The drinking water has become contaminated with lead in many countries across the world. In this study, a novel lead-imprinted polyvinylidene fluoride (PVDF) membrane was successfully fabricated for selective decontamination of lead from water. First of all, the membrane fabrication process was explored and optimized. The physical and chemical properties were then studied for a better understanding of the features of the membrane. The performance of lead removal by the adsorptive membrane was evaluated by systematic batch adsorption experiments, including pH effect, kinetics, isotherm, selectivity, and regeneration studies. The results indicated that the adsorptive membrane showed a high adsorption capacity of 40.59 mg Pb/g at the optimal pH of 5.5, fast kinetics of 2 h, high selectivity towards lead, and outstanding regeneration performance. The Langmuir equation fitted the isotherm better than the Freundlich equation, while the pseudo-second-order model and pore diffusion model well described the kinetics. The adsorptive membrane showed high selectivity towards lead in the lead/zinc binary solution. In the continuous filtration study, a small piece of adsorptive membrane could treat 3.75 L of lead solution. The XPS studies revealed that the lead uptake was mainly due to the complex reaction between lead and carboxyl and hydroxyl in the membrane.
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 28
·11486-11499
·
IF 4.5
Jiang Yanxiao,Song Wei,Zhang Meng,Feng Yu,Liu Boyan,Zhang Hong,Kan Guangfeng,Yu Kai,Jiang Jie
In this study, metal–organic framework (MOF)-functionalized sponge columns were prepared using a simple approach by embedding melamine sponge in a homogeneous MOF solution and first applied in the removal of methyl orange dye from water samples. Various MOF materials (MIL-101(Cr), MIL-101(Fe), ZIF-8(Zn), HKUST-1(Cu), and MIL-68(Al)) with different structures were synthesized and used as coating materials for a blank sponge. This method not only can be used for a wide variety of MOF materials, but also can retain their unique properties. The results show that the sponge as an adsorbed base material can effectively simplify the separation procedures of adsorption. Under the optimal conditions, the prepared MOF/PVDF-sponge column had an excellent adsorption capacity (229.4 mg g −1 ) toward methyl orange and reached the equilibrium within 1 h. With simple one-step infiltration, excellent adsorption properties and simple operation, the MOF/PVDF-sponge column presents a promising commercial value. Moreover, this study provides a new approach for exploring functional porous sponges for adsorption of dyes from environmental water samples.
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Science China-Technological Sciences
·
2023
·Vol. 66
·期 7
·2059-2068
·
IF 4.6
Gao Ling,Xie YuLin,Tong Yan,Xu Miao,You JiaLe,Wei HuiPing,Yu XiangXiang,Xu SiQi,Zhang Yi,Che Yong,Tang Ya,Suzuki Kota,Kanno Ryoji,Zhao GuoWei
Argyrodites, Li 6 PS 5 X ( X =Cl, Br, I), have piqued the interest of researchers by offering promising lithium ionic conductivity for their application in all-solid-state batteries (ASSBs). However, other than Li 6 PS 5 Cl (651Cl) and Li 6 PS 5 Br (651Br), Li 6 PS 5 I (651I) shows poor ionic conductivity (10 −7 S cm −1 at 298 K). Herein, we present Al-doped 651I with I − /S 2− site disordering to lower activation energy ( E a ) and improve ionic conductivity. They formed argyrodite-type solid solutions with a composition of (Li 6−3 x Al x )PS 5 I in 0⩽ x ⩽0.10, and structural analysis revealed that Al 3+ is located at Li sites. Also, the Al-doped samples contained anion I − /S 2− site disorders in the crystal structures and smaller lattice parameters than the non-doped samples. Impedance spectroscopy measurements indicated that Al-doping reduced the ionic diffusion barrier, E a , and increased the ionic conductivity to 10 −5 S cm −1 ; the (Li 5.7 Al 0.1 )PS 5 I had the highest ionic conductivity in the studied system, at 2.6×10 −5 S cm −1 . In a lab-scale ASSB, with (Li 5.7 Al 0.1 )PS 5 I functioned as a solid electrolyte, demonstrating the characteristics of a pure ionic conductor with negligible electronic conductivity. The evaluated ionic conduction is due to decreased Li + content and I − /S 2− disorder formation. Li-site cation doping enables an in-depth understanding of the structure and provides an additional approach to designing better-performing SEs in the argyrodite system.
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JOURNAL OF POLYMER RESEARCH
·
2022
·Vol. 29
·期 11
·1-14
·
IF 3.061
Zhang Zhao Xin,Yang Shang Ke,Shen Jun Wei,Yang Jia,Bian Jun,Zhang Ai Ping,Lin Hai Lan,Chen Dai Qiang
In order to systematically investigate the dependence of the properties of nanocomposites on the shape of nanofillers, including spherical and fibrous, and the contents and its special arrangement, polyimide (PI) as matrix, nano-silicon carbide particles (SiC p ) and whisker (SiC w ) as fillers were applied to prepare PI nanocomposite films by in-situ polymerization. FTIR and XRD tests verified the successful polymerization of SiC/PI nanocomposites. FESEM observations showed that both SiC p and SiC w nanofillers were uniformly dispersed in the PI matrix during in-situ polymerization and contributed to the improvements of properties. Compared with pure PI film, addition of SiC nanofillers enhanced obviously the heat resistance and the thermal stabilities of PI nanocomposites, as verified by TGA. Tensile tests indicated that the mechanical properties of PI nanocomposites enhanced with increasing SiC nanofillers. Moreover, SiC w was more prominent than SiC p in the reinforcement of PI nanocomposites. Due to the influences of dielectric properties by the changes of the spatial arrangement and the local distribution of electric field of the nanofillers in PI matrix, the dielectric constant of 3wt.%SiC p /PI and 3wt.%SiC w /PI nanocomposites reached 4.3 and 5.6, respectively. Compared with pure PI film, the dielectric constants of SiC p /PI and SiC w /PI nanocomposites were enhanced by 26% and 64%, respectively. In comparison, PI nanocomposites containing SiC w possessed higher effective permittivity than those containing SiC p under the same nanofillers concentration. This work is expected to show great significance to understand the microscopic mechanism of PI dielectric nanocomposites for high energy-storage applications.
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