ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Chuiyu Li,Zongqi Chen,Cuicui Zhou,Shiqi Hong,Songwang Yang
In the one-step solution method of perovskite film preparation, antisolvents are widely used to control perovskite crystallization, which directly influences the quality of the perovskite films. Herein, hexafluorobenzene (HFB) was involved in the mixed antisolvent (MAS) system to produce high-quality perovskite films with dual functions of crystallization control and defect passivation. Beyond improving perovskite crystallization and interface contact, a small amount of HFB remained in the perovskite and passivated uncoordinated Pb2+ defects. Consequently, the HFB-involved MAS-derived perovskite films exhibited higher crystallinity, smoother surfaces, better interfacial contacts, and fewer defects than those without HFB additives. These enhancements in film quality significantly improved the open-circuit voltage (VOC) and the fill factor (FF) of the corresponding solar cells, resulting in an increase in power conversion efficiency (PCE) from 23.18% to 24.53%. Furthermore, the solar cells prepared by this method exhibited improved stability. This study highlights a facile and efficient method for simultaneously regulating perovskite crystallization and mitigating defects by incorporating functionalized mixed antisolvents, thus improving the photovoltaic performance of perovskite solar cells.
研究领域:
材料科学
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能源科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
TETRAHEDRON
·
2014
·
IF 2.817
Junchao Xu,Leiming Zhu,Qiusheng Wang,Lintao Zeng,Xichao Hu,Boqiao Fu,Zhe Sun
A series of meso -C 6 F 5 BODIYs have been successfully synthesized and characterized. Some of them displayed excellent spectroscopic properties, such as relatively large Stokes shift , high fluorescence quantum yield , far-red or near infrared region (NIR) emission, and good photostability. In particular, the dye functionalized with oligo(ethylene glycol) ether-phenyl groups at the 3,5-position of BODIPY core became water-soluble and its emission located in the NIR region with large Stokes shift. Time-dependent density functional theory calculations were conducted to understand the structure–optical properties relationship. Furthermore, cell staining tests demonstrated that the meso -C 6 F 5 BODPY derivative with oligo(ethylene glycol) ether-phenyl group was membrane permeable and selectively stained cytosol in living cells.
研究领域:
化学
·
生物医学工程
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细胞生物学
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产品关联
DOI
高影响因子
PESTICIDE BIOCHEMISTRY AND PHYSIOLOGY
·
2024
·
IF 4.2
Yu-Juan Yao,Ning-Na Yin,Lin-Mei Pu,An-Jing Yang,Nai-Yong Liu
Antennae and legs (primarily the tarsal segments) of insects are the foremost sensory organs that contact a diverse range of toxic chemicals including insecticides. Binding proteins expressed in the two tissues are potential molecular candidates serving as the binding and sequestering of insecticides, like chemosensory proteins (CSPs). Insect CSPs endowed with multiple roles have been suggested to participate in insecticide resistance , focusing mainly on moths, aphids and mosquitos. Yet, the molecular underpinnings underlying the interactions of cerambycid CSPs and insecticides remain unexplored. Here, we present binding properties of three antenna- and tarsus-enriched RhorCSPs (RhorCSP1, CSP2 and CSP3) in Rhaphuma horsfieldi to eight insecticide classes totaling 15 chemicals. From the transcriptome of this beetle, totally 16 CSP-coding genes were found, with seven full-length sequences. In phylogeny, these RhorCSPs were distributed dispersedly in different clades. Expression profiles revealed the abundant expression of RhorCSP1 , CSP2 and CSP3 in antennae and tarsi, thus as representatives for studying the protein-insecticide interactions. Binding assays showed that the three RhorCSPs were tuned differentially to insecticides but exhibited the highest affinities with hexaflumuron, chlorpyrifos and rotenone (dissociation constants <13 μM). In particular, RhorCSP3 could interact strongly with 10 of tested insecticides, of which four residues (Tyr25, Phe42, Val65 and Phe68) contributed significantly to the binding of six, four, three and four ligands, respectively. Of these, the binding of four mutated RhorCSP3s to a botanical insecticide rotenone was significantly weakened compared to the wildtype protein. Furthermore, we also evidenced that RhorCSP3 was a broadly-tuned carrier protein in response to a wide variety of plant odorants outside insecticides. Altogether, our findings shed light on different binding mechanisms and odorant-tuning profiles of three RhorCSPs in R. horsfieldi and identify key residues of the RhorCSP3-insecticide interactions.
研究领域:
昆虫学
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分子生物学
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生物化学
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昆虫毒理学
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DOI
PubMed
高影响因子
JOURNAL OF MEMBRANE SCIENCE
·
2024
·
IF 8.4
Jiaqi Shuai,Shengqiu Zhao,Yucong Liao,Fanglin Wu,Rui Wang,Letian Wang,Chunhui Shen,Haolin Tang
Ammonia as a hydrogen enrichment medium has tremendous advantages over pure hydrogen in terms of transportation and utilization. The high-efficiency anti-ammonia-poisoning membrane electrode assembly (MEA) is pivotal for the practical implementation of ammonia-resistant proton exchange membrane fuel cells (PEMFCs). As for the polymer electrolyte, which is an integral part of the proton exchange membrane (PEM) and catalyst layer (CL) adhesion agents in the MEA, structural design is an effective way to improve its resistance to ammonia poisoning. Herein, an in-depth study of sulfonimides with superacidic structures reveals that the proton dissociation energies can be altered by tuning the terminal groups with different electronegativity and enhancing the competitive adsorption of protons on Pt. Four perfluorinated backbone sulfonimides (PFSI-x (x = TSM, MSA, ESA, and iPSA)) with distinct charge delocalization were fabricated by grafting different electronegative monomers onto the perfluorosulfonyl fluoride (PFSF). The results show that PFSI-TSM possesses a higher electrostatic potential (2.69 eV) and the lowest activation energy (12.1 kJ/mol). Meanwhile, the performance of the PFSI-TSM PEMFC is 40.6% higher than the perfluorosulfonic acid (PFSA) at 80 °C, 100% relative humidity (RH) under 100 ppm NH 3 , with a maximum power density of 635.2 mW/cm 2 . The underlying reason for enhanced performance is in virtue of the more electronegative end groups render the superacid electrolyte with higher acidity and p K a values, which change the direction of the acid dissociation equilibrium reaction on the Pt surface, enhanced competitive adsorption of protons in MEAs elevated oxygen reduction reaction (ORR) activity and proton concentration in PEM and reduced the probability of ammonia adsorption poisoning. The insights in charge delocalization and proton ionization construct the structure-property relationship, which would guide a rational design of PEM for ammonia-resistant fuel cells.
研究领域:
材料科学
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能源工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Yucong Liao,Shengqiu Zhao,Guoliang Liu,Hao Li,Jiaqi Shuai,Letian Wang,Bingxuan Liu,Haolin Tang
Proton exchange membrane fuel cells (PEMFCs) face a significant challenge when operating in high-temperature and low-humidity environments, the hydrocarbon-based polymers that are sulfonated or phosphonated can’t meet the demand for achieving high performance. Modifying perfluorosulfonyl fluoride (PFSF) through meticulous design of side-chain chemical structures and introducing functionalized sulfonimide and phosphonic acid groups. Membranes derived from a perfluorocarbon backbone and polyacid side chain structures exhibit distinct microphase separation. The sulfonimide group exhibits hyper-acidic properties, whereas the phosphonic acid group functions as proton acceptor and donor. These two groups work synergistically to establish a distinct proton transport channel. The robust adsorption between acidic functional groups and water molecules enhances the diffusion of water molecules, resulting in an increase in proton conductivity. Moreover, Density Functional Theory (DFT) calculations reveal that the phosphonic acid group of the side chain has difficulty forming anhydrides. The prepared perfluorosulfonimide-phosphonic acid (PFSNPA) proton exchange membrane demonstrates an impressive conductivity of 263 mS·cm −1 at 120 °C. In H 2 /Air fuel cell tests, PFSNPA achieves an outstanding output power of 1076.1 mW·cm −2 at 120 °C and 40 % RH. This study introduces a new approach for designing and fabricating proton exchange membrane materials for high-temperature fuel cells.
研究领域:
材料科学
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能源工程
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产品关联
DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Cairong Wang,Yao Tong,Yadong Wang,Haolin Tang,Haining Zhang
Improving the oxygen transport ability without sacrificing proton conductivity in cathode catalyst layer is an essential way to increase the performance, thereby reducing platinum usage of proton exchange membrane fuel cells (PEMFCs). Herein, we report the influence of equivalent weight of dioxole-contained highly oxygen permeable perfluorosulfonic acid ionomers as catalyst binder and proton conductor in cathode catalyst layer on the performance of PEMFC. The results reveal that the increase in the fraction of dioxole segments leads to the enhanced oxygen permeation but the decreased proton conductivity in catalyst layer. With optimization of equivalent weight of the synthesized ionomers, the accordingly assembled cell with platinum loading of 0.125 mg cm −2 for both anode and cathode exhibits an improved concentration polarization, leading to an increased peak power density by 166 mW cm −2 at current density of 2900 mA cm −2 compared to Nafion ionomer-based PEMFC at 2800 mA cm −2 using hydrogen and air as reactant gases.
研究领域:
化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Runqiao Hou,Yuchen Yang,Kaixin Ren,Shouyi Yuan,Yonggang Wang
Batteries with Li metal anodes are promising to achieve ultrahigh energy densities over 500 Wh kg–1. However, Li dendrite growth and related issues hinder their practical application. Although strategies like “salt-in-solvent” and “weakly solvating” approaches have been successfully demonstrated to suppress the dendrite growth and achieve high energy densities by enhancing the oxidative tolerance of ethereal electrolytes, they often compromise Li+ dissociation, thus undermining their fast-charging performance. Herein, we propose a synergic regulation strategy of Li+ desolvation kinetic and Li metal interfacial chemistry via the addition of hexafluorobenzene (HFB) and ionic liquid (N-propyl-N-methylpyrrolidinium nitrate (Py13NO3)). In this electrolyte, NO3– and FSI– anions penetrates into the inner solvation shell of Li+, weakening the solvation strength of 1,2-Dimethoxyethane (DME), meanwhile, the Py13+ drags the FSI–, NO3– anions and the DME, thus prompting the desolvation process of Li+. Meanwhile, the interfacial adsorption of HFB facilitates the formation of a LiF-rich interphase with improved ionic conductivity. Consequently, the electrolyte containing 2 M LiFSI 0.3 M Py13NO3 in DME/HFB (9/1, v/v) demonstrates excellent cycling stability in high-voltage Li || NCM811 cells, maintaining 83.8% capacity retention over 800 cycles at a high rate of 5 C. Notably, even under a stringent negative/positive capacity (N/P) ratio of 1, the capacity retention of 82.1% is still retained after 100 cycles.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
IF 14.7
Liu Cong,Mei Bingbao,Shi Zhaoping,Jiang Zheng,Ge Junjie,Xing Wei,Song Ping,Xu Weilin
Heterogeneous nano-electrocatalysts doped with nonmetal atoms have been studied extensively based on the so-called dopant-based active sites, while little attention has been paid to the stability of these dopants under working conditions. In this work, we reveal significantly, when the redox working potential is too low negatively or too high positively, the active sites based on these dopants actually tend to collapse. It means that some previously observed “remarkable catalytic performance” actually originated from some unknown active sites formed in situ. Take the Bi-F for the CO 2 RR as an example, results show that the observed remarkable activity and stability were not directly from F-based active sites, but the defective Bi sites formed in situ after the dopant leaching. Such a fact is unveiled from several heteroatom-doped nanocatalysts for four typical reactions (CO 2 RR, HER, ORR, and OER). This work provides insight into the role of dopants in electrocatalysis.
研究领域:
电化学
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催化
·
材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF POWER SOURCES
·
2018
·
IF 6.945
Yuanfang Hu,Bingxi Wang,Xiao Li,Dongyang Chen,Weiying Zhang
To develop high performance anion exchange membranes (AEMs), a novel bisphenol monomer bearing eight benzylmethyl groups at the outer edge of the molecule was synthesized, which after condensation polymerization with various amounts of 4,4′-dihydroxydiphenylsulfone and 4,4′-difluorobenzophenone yielded novel poly(arylene ether)s with densely located benzylmethyl groups. These benzylmethyl groups were then converted to quaternary ammonium groups by radical-initiated bromination and quaternization in tandem, leading to the emergence of densely quaternized poly(arylene ether sulfone)s (QA-PAEs) with controlled ion exchange capacities (IECs) ranging from 1.61 to 2.32 mmol g −1 . Both small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM) studies revealed distinct phase separation in the QA-PAEs. The QA-PAE-40 with an IEC of 2.32 mmol g −1 exhibited a Br − conductivity of 9.2 mS cm −1 and a SO 4 2− conductivity of 14.0 mS cm −1 at room temperature , much higher than those of a control membrane with a similar IEC but without obvious phase separation. Therefore, phase separation of AEMs was validated to be advantageous for the efficient conducting of anions. The experimental results also showed that the QA-PAEs were promising AEM materials, especially for non-alkaline applications.
研究领域:
材料科学
·
化学工程
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产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2017
·
IF 6.395
Chen Xiao Lin,Xiu Qin Wang,Ling Li,Fang Hua Liu,Qiu Gen Zhang,Ai Mei Zhu,Qing Lin Liu
To explore highly conductive and alkaline stable anion exchange membrane (AEM) materials, triblock copolymers bearing alkyl-tethered cycloaliphatic quaternary ammonium-head-groups are prepared via nucleophilic substitution , Friedel-Crafts acylation, ketone reduction and Menshutkin reaction . The designed triblock copolymers composed of quaternized poly(phenylene oxide) segments and poly(ether sulfone) segments are responsible for the microphase separated morphology and well-connected ion domains, as confirmed by transmission electron microscopy . The highest conductivity, up to 105.1 mS cm −1 at 80 °C is achieved for the AEM with ionic exchange capacity (IEC) of 1.81 meq g −1 . Furthermore, the AEMs show robust alkaline stability due to the alkyl-tethered cation-head-groups structure. High retention of hydroxide conductivity (88.9%) and IEC (91.2%) is observed for the AEMs via degradation test in a 1 M aqueous KOH solution at 80 °C for 480 h. Based on the AEM with high conductivity, a H 2 /O 2 fuel cell achieves a peak power density of 176.5 mW cm −2 (80 °C) at a current density of 500 mA cm −2 .
研究领域:
材料科学
·
燃料电池技术
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产品关联
DOI
高影响因子
BIOMACROMOLECULES
·
2022
·
IF 6.978
Fei Fu,Minggui Shen,Dan Wang,He Liu,Shibin Shang,Fei-Long Hu,Zhanqian Song,Jie Song
Low-k dielectrics are urgently needed in modern integrated circuits. The introduction of free volume instead of porous structures has become a powerful strategy to reduce the k value. According to this strategy, the biomass resource rosin-containing hydrogenated phenanthrene ring was introduced into benzocyclobutene (BCB) resin to reduce the k value; then a rosin-based BCB monomer was successfully synthesized. Meanwhile, the BCB monomer without a rosin skeleton was prepared. After converting the monomers into thermo-crosslinked materials, notably that the rosin skeleton has a great influence on the free volume and k value of the material. The fractional free volume and k value of the former are 26% and 2.44, respectively, and those of the latter are 14% and 2.84, respectively. In addition, the distances between molecular chains and the density of the former are 0.60 nm and 1.06 g cm–3, respectively; those of the latter are 0.56 nm and 1.28 g cm–3, respectively. These data show that introducing hydrogenated phenanthrene rings occupies part of the space and hinders the packing of molecular chains, which increases the distance between molecular chains and reduces the density of the polymer, resulting in an increasing free volume and a reducing k value. Notably that introducing hydrogenated phenanthrene rings cannot affect other properties of the material. Therefore, this research indicates that introducing rosin skeletons can prepare high-performance materials, which provide some promising low-k materials for the development of electronics and microelectronics.
研究领域:
材料科学
·
电子工程
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2022
·
IF 4.601
Yanyan Wang,Liuqian Bao,Jiajing Sun,Yuanyuan Ding,Jiasheng Shi,Zhengyu Duan,Zhiyong Chen
Fluorous affinity chromatography has received growing attention in separation and purification of fluoro compounds, but the wettability of the fluorinated stationary phases is seldom noticed. Here, we construct a series of micro-sized fluorine-containing microspheres by solvothermal precipitation polymerization. The fluorinated microspheres could be obtained with narrow size distribution at even high monomer loading of 15 wt%. Through alternating fluoro monomer, both the particle size and the wettability of the microsphere array could be tuned. Among them, the poly(divinylbenzene -dodecafluoroheptyl methacrylate), P(DVB-DFHMA), microsphere (6.1 μm) arrays displays superhydrophobicity with 153.2° water contact angle. The P(DVB-DFHMA) fluorinated microspheres (7.58% fluorine content) can be packed into steel-less columns as stationary phase for high-performance liquid chromatography. The retention mechanism of the fluorinated column is proven to be the specific fluorine-fluorine interaction. Compared to the commercial C18 silica column, the fluorinated column can completely separate fluorine-containing compounds under high water content mobile phase, including small fluoro molecules and fluoro macromolecules, at much lower back pressure by fluorous affinity.
研究领域:
化学
·
材料科学
·
分析化学
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产品关联
DOI
PubMed
高影响因子