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ACS Applied Nano Materials · 2021 · IF 5.097

V2CTx and Ti3C2Tx MXenes Nanosheets for Gas Sensing

Meng Wu,Yipeng An,Ru Yang,Zhenhua Tao,Qixun Xia,Qianku Hu,Mian Li,Ke Chen,Zhanying Zhang,Qing Huang,Shu-hong Ma,Aiguo Zhou

In this paper, the performance and fundamental mechanisms on gas sensing of V2CTx and Ti3C2Tx MXenes were investigated. The MXenes nanosheets with the same chemical composition can show positive or negative response to the same gas due to the change of surface chemistry, which, in turn, is affected by the etching solution to make the samples. The residual Li or Na atoms on the surface of MXenes have a weak impact on the gas sensing performance; however, the ratio of Cl/F has a strong impact. V2CTx made in HF showed positive/zero response to the eight gases tested in this paper and had excellent sensing performance to methane. However, V2CTx made in LiF+HCl showed negative/zero response, while that made in NaF+HCl displayed positive response only to formaldehyde. Ti3C2Tx made in NaF+HCl showed a positive response to all detected gases while that made in ZnCl2 had better gas detection ability but showed a negative response to ammonia, triethylamine, and toluene. On the basis of the theoretical simulations, the structure-sensitive sensing behavior of MXenes as gas sensors is mainly ascribed to the structure-dependent electron transmission mechanism upon adsorbed gas molecule. This study is significant to the application of MXene sensors for designing specific gases.

CAS / MDL: 7664-39-3 7789-24-4
研究领域: 材料科学 · 化学
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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Near infrared light responsive surface with self-healing superhydrophobicity in surface chemistry and microstructure

Yacong Hou,Ding Weng,Yadong Yu,Jiadao Wang,Lei Chen

Self-healing superhydrophobic surfaces have attracted considerable attention for enhancing the durability of superhydrophobic coatings, which have applications in various fields. However, it is difficult to find safe and effective strategies for self-healing superhydrophobic coatings to recover both microstructure and surface chemistry simultaneously. Herein, we demonstrate a high-efficiency self-healing hydrophobic surface with remote control ability. Through near infrared light (NIR) irradiation, the collapsed surface microstructure and altered surface chemistry can be recovered easily and simultaneously in a very short period. The extraordinary performance is fully discussed and can be attributed to the excellent photothermal properties of candle soot (CS). In addition, the surface demonstrates repeatable self-healing ability thanks to the good shape memory of the epoxy-based shape memory polymer (SMP) and the continued release of fluorinated alkyl silane encapsulated in microcapsules. The presented surface shows great potential and broad impacts owing to its simplicity and efficiency.

研究领域: 材料科学 · 表面化学
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Quasi-In Situ XPS Insights into the Surface Chemistry of Garnet-Type Li6.4La3Zr1.4Ta0.6O12 Solid-State Electrolytes: The Overlooked Impact of Pretreatments and a Direct Observation of the Formation of LiOH

Yifan Zhou,Aosong Gao,Mingqiu Duan,Xiaoqi Zhang,Muzi Yang,Li Gong,Jian Chen,Shuqin Song,Fangyan Xie,Hao Jia,Yi Wang

Garnet-type Li6.4La3Zr1.4Ta0.6O12 (LLZTO) is a highly promising solid-state lithium metal battery electrolyte due to its exceptional ionic conductivity and electrochemical stability. However, when exposed to air, a passivation layer can be spontaneously formed on the garnet-type electrolyte, deteriorating its wettability with metallic lithium (Li) and impeding the lithium ion transfer at the Li–garnet electrolyte interface. The passivation layer is considered a critical issue for garnet-type solid electrolytes. Despite intensive research, the formation mechanism of the passivation film remains poorly understood. The key to elucidating the formation mechanism is to obtain a pristine garnet electrolyte surface and study how the pristine garnet electrolyte interacts with air. In this study, different passivation layer removal pretreatments were performed to expose pristine garnet electrolytes, and their impacts on the samples were systematically studied. The results reveal the overlooked negative impacts of vacuum annealing and acid treatment on LLZTO, which are indicated by the severe loss of Li and O and the formation of additional Li-depleted metal oxides. It was confirmed that argon annealing is the only viable approach to remove the passivation layer without introducing concomitant contaminations to LLZTO. Based on this method, we directly evidenced the formation of LiOH on LLZTO under rarefied air using quasi-in situ X-ray photoelectron spectroscopy. It was confirmed that the loss of Li and O ions, rather than Li+/H+ exchange, drives the formation of LiOH in the passivation layer. These results not only provide a better understanding of the surface and interface chemistry of LLZTO but also reveal a reliable surface treatment for the LLZTO sample.

CAS / MDL: 1314-23-4 1314-61-0
研究领域: 材料科学 · 电化学
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JOURNAL OF FLUORINE CHEMISTRY · 2018 · IF 1.879

Fabrication of self-assembled hydrophobic fluorinated silica particulate film

Yudi Guo,Erqing Zhao,Xiaowei Guo,Dongyan Tang

Hydrophobic fluorinated particulate films were fabricated by coupling Langmuir-Blodgett silica (LB-SiO 2 ) particulate monolayers with fluoroacrylate polymer, and the depth distributions of chemical compositions were studied. The resultant fluorinated particulate films show surface hydrophobic property with water contact angles (WCA) of 123° (300 nm) and 125° (550 nm), which is dominated in Wenzel wetting state. The surface F/C ratio is only 0.09 at 20°, which is slightly higher than 0.07 at 60°. Fitting results of C1s and O1s high-resolution spectra at 20° and 60° indicate the outmost surface is mainly occupied by fluoroacrylate polymer main chains and the ester side chains stretch toward inner surface and thus hydrophobic fluorinated groups in self-assembled fluoroacrylate film cannot efficiently segregate to the outer surface, which results in low surface F/C ratio and surface WCA.

研究领域: 材料科学 · 表面化学
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ADVANCED FUNCTIONAL MATERIALS · 2022 ·Vol. 33 ·期 3 ·2211335 · IF 19.924

Surface Chemistry Determined Electrochemical Sensing Performance of Red Phosphorus and Single Walled Carbon Nanotube Composites

Lingbo Liu,Ling Lei,Keni Zeng,Kangbing Wu,Nianjun Yang

Red phosphorus (RP) is a promising electrochemical sensing material owing to its abundant surface groups and reactive sites. In this study, a sodium dodecyl sulfate-assisted phosphorus-amine approach is employed to tune surface chemistry of RP nanoparticles. During the transition of the polyphosphorus-amine anion to RP, the cleavage of P  O  P bond and the formation of P  O  C bond are monitored by in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy. The formed P  O  C bonds that are originated from the P  O  reactive sites are theoretically revealed with the density functional theory calculations, charge density difference, and X-ray photoelectron spectroscopy. The energies of optimized aromatic and aliphatic P  O  C bonds are −2.51 and −2.65 eV, respectively. To explore electrochemical sensing applications, RP nanoparticles are in situ grown on single-walled carbon nanotube (SWCNT). Such a stable RP/SWCNT suspension is applied to fabricate the RP/SWCNT integrated arrays via a template-filtration method. Such an array is efficient for sensitive and selective monitoring of p-phenylenediamine on hair dyes. This study provides insights into surface chemistry of RP, its roles in electrochemical sensing applications, and an approach to produce high-performance RP sensors at large scales.

CAS / MDL: 107-15-3
研究领域: 材料科学 · 电化学 · 表面化学
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LANGMUIR · 2018 · IF 3.789

Co-deposition Kinetics of Polydopamine/Polyethyleneimine Coatings: Effects of Solution Composition and Substrate Surface

Yan Lv,Shang-Jin Yang,Yong Du,Hao-Cheng Yang,Zhi-Kang Xu

Polydopamine-based chemistry has been employed for various surface modifications attributed to the advantages of universality, versatility, and simplicity. Co-deposition of polydopamine (PDA) with polyethyleneimine (PEI) has then been proposed to realize one-step fabrication of functional coatings with improved morphology uniformity, surface hydrophilicity, and chemical stability. Herein, we report the co-deposition kinetics related to the solution composition with different dopamine/PEI ratios, PEI molecular weights, dopamine/PEI concentrations, and the substrate surface with varying chemistry and wettability. The addition of PEI to dopamine solution suppresses the precipitation of PDA aggregates, resulting in an expanded time window of steady co-deposition compared with that of PDA deposition. Low-molecular-weight PEI at low concentration accelerates the co-deposition process, while high-molecular-weight PEI and high concentration of either PEI or dopamine/PEI are detrimental to the co-deposition efficiency. Meanwhile, the surface morphology and chemical composition of the co-deposition coatings can be regulated by the solution conditions during co-deposition. Moreover, obvious deviations in the co-deposition rate and the amount of substrates bearing various functional groups, such as alkyl, phenyl, hydroxyl, and carboxyl, are revealed, which are quite different from PDA deposition. The initial adsorption rates further reflect the change in interactions between the aggregates and these substrates caused by PEI, which follows the sequence of carboxyl > hydroxyl > alkyl > phenyl. These results provide deep insights into the PDA/PEI co-deposition process on various substrates.

CAS / MDL: 9002-98-6
研究领域: 材料科学 · 表面化学 · 生物医学工程
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Surface chemical engineering towards efficient and bright chemiluminescent carbon nanodots

Cheng-Long Shen,Jin-Hao Zang,Qing Lou,Guang-Song Zheng,Meng-Yuan Wu,Yang-Li Ye,Jin-Yang Zhu,Kai-Kai Liu,Lin Dong,Chong-Xin Shan

Carbon nanodots (CDs) are emerging as low toxic chemiluminescent (CL) materials for new-generation cold lighting and bioimaging technology due to their tunable and efficient emissions. Nevertheless, continuous progress and efforts are still needed to improve the luminance and lifetime of the CL CDs. Here, CL quenching is observed in the CD-peroxyoxalate-hydrogen peroxide system, resulting from the water-induced aggregation and blocking effect of the electron exchange between the CDs and energetic intermediate produced in the CL reaction. A surface chemical regulation strategy is first introduced to improve the CL performance of CDs. Optimized the capped ligand species and chain length, the CDs modified by n-butylamine exhibit a CL quantum yield of 1.15 × 10 –2 einsteins mol −1 and maximal luminance of 5.11 cd m −2 , which is about 5- and 13-fold higher than the initial CDs and comparable with commercially available Rhodamine B. The enhanced performance can be explained by the decreased electron capture from water molecules generated due to the decomposition of hydrogen peroxide in the CL process.

研究领域: 材料科学 · 化学工程 · 生物成像
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COMPOSITES PART A-APPLIED SCIENCE AND MANUFACTURING · 2019 · IF 6.282

Interfacial adhesion between carbon fibers and nylon 6: Effect of fiber surface chemistry and grafting of nano-SiO2

Tao Zhang,Yue Xu,Hongfu Li,Boming Zhang

In this study, the effect of carbon fiber (CF) surface chemistry and grafting of nano-SiO 2 on CF surface with respect to the interfacial adhesion of CF-reinforced nylon 6 composites was investigated. CFs were oxidized and reacted with poly(oxypropylene) diamines to modify the surface chemistry. The oxidized CFs were modified with 3-aminopropyltriethoxysilane and then grafted with SiO 2 nanoparticles. Fourier transform infrared spectroscopy (FT-IR), X-ray photoelectron spectroscopy (XPS), scanning electron microcopy (SEM), and atomic force microscopy (AFM) were used to characterize the chemistry and topographies of the CF surface. The transverse fiber bundle strength of CF oxidized and grafted nano-SiO 2 increased to 31.92 MPa and 39.35 MPa, respectively, from 12.57 MPa for untreated CF. The results indicated that the reaction between the carboxyl group and nylon 6 led to chemical bonding at the interface and it meanwhile was strengthened and toughened by uniformly distributed SiO 2 nanoparticles on the CF surface.

研究领域: 材料科学 · 复合材料
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CHEMICAL ENGINEERING JOURNAL · 2023 · IF 15.1

Hydrogen bonding donor/acceptor active sites exposed on imide-functionalized carbon dots aid in enhancing arsenic adsorption performance

Ze Lin,Limin Jin,Yanbiao Liu,Ying Wang

During the arsenic (As) adsorption process, amino-functionalization has been widely considered as one of the effective adsorbents optimization methods, while this study reveals that imide functional groups also play a non-negligible role. Herein, magnetic carbon dots (CDs) equipped with imide (FeCD-NH) or amino functional groups (FeCD-NH 2 ) were synthesized to deduce the relationship between different configurations of amino-like functional groups and As. The results showed that FeCD-NH exhibited extraordinary As(V) adsorption behavior (with 97.80 % As(V) removal within 5 min), outperformed that equipped with amino functional groups (FeCD-NH 2 ). An array of advanced characterization techniques and density functional theory (DFT) calculation collectively revealed a dual-configuration hydrogen bond synergistic mechanism of FeCD-NH toward As(V). Different from monomorphic hydrogen bond of amino functional group, imide functional group forms abundant adsorption sites through dual-configuration hydrogen bonds to realize the ultrafast adsorption of As(V). In addition, FeCD-NH can remove As(V) from other more complex water matrices to levels below the World Health Organization (WHO) drinking water standards and the Chinese surface water standards. Therefore, this work provides a promising strategy for As decontamination by fine-tune the surface chemistry of adsorbents.

CAS / MDL: 541-59-3
研究领域: 环境科学 · 材料科学
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GREEN CHEMISTRY · 2023 ·Vol. 26 ·期 3 ·1627-1636 · IF 9.8

Effective flotation separation of apatite from dolomite using a new eco-friendly depressant gallic acid

Shengzong Lan,Peilun Shen,Qifang Zheng,Lidong Qiao,Liuyang Dong,Dianwen Liu

Apatite and dolomite present challenges in their separation due to their similar surface chemistry. To achieve flotation separation of apatite and dolomite, depressants are required, but conventional depressants have several drawbacks. Hence, the development of effective and environmentally friendly depressants is of great importance. This study aimed to investigate the depressive effect of gallic acid (GA) on the flotation separation of apatite from dolomite using sodium oleate (NaOL) as the collector. The floatability of apatite and dolomite was examined through micro-flotation. The findings revealed that, with 1.0 × 10−4 mol L−1 NaOL, the recovery rates of apatite and dolomite were 86.29% and 77.42%, respectively. After introducing 2.0 × 10−4 mol L−1 GA, the recovery of apatite remained at 83.42%, while that of dolomite drastically decreased to only 14.33%. The selective depression mechanism of GA in the flotation separation of apatite from dolomite was investigated using various techniques, including zeta potential, contact angle, UV-vis, FTIR, XPS, ToF-SIMS, and AFM analyses. The results demonstrated that GA increased the hydrophilicity of the dolomite surface and impeded the adsorption of NaOL on that surface without affecting the apatite. GA was found to bind to Ca and Mg sites on the dolomite surface through –OH and –COOH groups. The adsorption of GA on the dolomite surface was substantial, with the adsorption height primarily concentrated in the range of 10–30 nm. GA exhibited selective depression on dolomite, thus, enabling successful flotation separation of apatite from dolomite.

CAS / MDL: 7440-55-3
研究领域: 矿物加工工程 · 环境科学
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CHEMISTRY OF MATERIALS · 2020 · IF 9.567

Stabilizing Na3Zr2Si2PO12/Na Interfacial Performance by Introducing a Clean and Na-Deficient Surface

Zhonghui Gao,Jiayi Yang,Haiyang Yuan,Haoyu Fu,Yutao Li,Yuyu Li,Thimo Ferber,Conrad Guhl,Huabin Sun,Wolfram Jaegermann,René Hausbrand,Yunhui Huang

Most Li+/Na+-conducting solid electrolytes are unstable in moisture, and the formed hydroxides and carbonates on their surfaces result in the increase of the interfacial resistance between solid electrolytes and alkali metal anodes. In this study, heat treatment was used to remove the byproduct coating on the surface of Na3Zr2Si2PO12 (NZSP) that also leads to the generation of Na-ion deficient surface simultaneously. This surface chemistry approach was used to reduce the interfacial resistance and suppress Na-dendrite growth during Na plating. A combination of the metallic Na wetting test, density functional theory, and electrochemical measurement was employed to investigate the origins of ultralow interfacial resistance and mechanism between the Na-ion deficient surface and the metallic Na anode. The analysis demonstrates that the Na-ion-deficient surface effectively improves the contact between NZSP and the metallic Na anode. Moreover, an ultrathin passivating layer involving Na2O was formed between NZSP with metallic Na that protected the NZSP electrolyte from the reduction by metallic Na. This study not only motivates the need for further understanding of the surface chemistry of NZSP but also provides guidelines for the future design of the Na-ion solid–electrolyte interface.

研究领域: 材料科学 · 电化学
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Toxicology Research · 2017 ·Vol. 6 ·期 5 ·693-704 · IF 1.969

Biological behaviors and chemical fates of Ag2Se quantum dots in vivo: the effect of surface chemistry

Tang Huan,Yang Sheng-Tao,Ke Da-Ming,Yang Yi-Fan,Liu Jia-Hui,Chen Xing,Wang Haifang,Liu Yuanfang

Ag2Se quantum dots (QDs) are novel fluorescent probes in the second near-infrared window with great imaging quality and biocompatibility. Surface modification is an essential step to disperse Ag2Se QDs into biological fluids, and endow Ag2Se QDs with diverse surface chemistry. However, the effect of surface chemistry on the biological behaviors and chemical fates of Ag2Se QDs has not been studied, which hinders the design of suitable Ag2Se QDs for biomedical applications. Here, the distribution, degradation, excretion and toxicity of 2-aminoethanethiol and mercaptopropionic acid coated Ag2Se QDs (denoted as QDs-MEA and QDs-MPA, respectively) were systematically investigated in mice for a 28-day observation period after a single intravenous injection. Ag2Se QDs with different surface chemistries displayed similar trends in all observations, such as fast blood clearance, main uptake in the liver and spleen, severe biotransformation, Ag excretion through feces, and low toxicity. The major different behaviors observed were the partially pulmonary deposition, the faster transformation at the initial stage, the lower excretion percentage, and the more obvious damage to the liver by QDs-MEA compared to QDs-MPA. The surface chemistry of Ag2Se QDs regulated their biological behaviors and chemical fates in vivo, and surface chemistry should be fully regarded when designing Ag2Se QDs for biomedical applications from the biosafety perspective.

研究领域: 生物医学 · 纳米材料科学
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