Journal of the American Chemical Society
·
2021
·
IF 15.419
Na Qu,Zhang Luo,Shuping Zhao,Bing Liu
Anisotropic colloidal particles are important building blocks for the studies of self-assembly, which are visualized models for basic research and can be used to construct structured materials. Discs are one of the most typical anisotropic colloids; however, the synthesis of monodisperse colloidal discs with well-defined shape remains a challenge. Here we report a novel strategy for synthesizing polymeric discs based on frame-guided droplet shrinkage. This was realized by creating frame/liquid core/shell rings and utilizing the shrinking instability of the liquid rings. The resulting disc’s shape parameters are tunable. The method is general, is not limited to specific polymers, solvents, and frames, and therefore has the potential to afford a variety of polymer discs. We also demonstrate the possibility of tuning the surface chemistry of the discs through surface-initiated polymerization. The frame-guided droplet shrinkage method opens up a new way to design and fabricate colloidal particles.
研究领域:
材料科学
·
化学工程
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DOI
高影响因子
Nanoscale
·
2021
·Vol. 13
·期 48
·20521-20530
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IF 7.79
Feiyu Zheng,Yingyue Zhang,Liuchang Dong,Dengwu Zhao,Rui Feng,Peng Tao,Wen Shang,Benwei Fu,Chengyi Song,Tao Deng
This paper reports an interfacial evaporation-driven approach for self-assembly of a gold nanoparticle (AuNP) film at the interface of liquid/air. We have designed colloidal plasmonic AuNPs capped with different types and surface coverage densities of ligands (i.e. purified and unpurified oleylamine-capped or thiol-protected AuNPs) and studied the impact of surface chemistry on the self-assembly of AuNPs using the optically excited plasmonic heating effect. By employing the extended DerjaguinLandau–Verwey–Overbeek model, the calculated lowest potential energies of the assembled AuNPs capped with purified oleylamine or alkyl thiols are between −1 kBT and −2 kBT, which is close to the room temperature thermal energy and represents a meta-stable assembly, indicating the reversible self-assembly of the AuNP film observed from the experiment. Furthermore, we observed the superheating phenomenon in well-dispersed nanoparticle solution while normal boiling occurred in the solutions with AuNP assemblies. The SERS activity of the as-prepared AuNP film has also been studied using rhodamine 6G as a molecular probe. This work not only provides a new aspect of the boiling phenomena of optically heated colloidal plasmonic nanoparticle solutions, but also provides inspiration for a new approach in designing surface ligands on the nanoparticles to realize reversible self-assembly via interfacial evaporation.
研究领域:
材料科学
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纳米技术
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光学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
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2024
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IF 6.7
Ge Guo,Yunsheng Xia
Carbon dot (C-dot) separation/purification is not only a fundamental chemical issue but also an essential precondition for revealing C-dots’ true nature. To date, adequate separation of C-dots has remained an open question due to the lack of an appropriate fine separation system. Herein, we discover and reveal that polyamide chromatography can provide versatile and powerful performances for C-dot separation. By a joint study of experiments and all-atom molecular dynamics simulations, we demonstrate that multiple interaction forces, including electrostatic repulsion/attraction, hydrogen bond, and van der Waals effects, exist simultaneously among the stationary phase, mobile phase, and the separated C-dots. Furthermore, the magnitude of these forces is dependent on the surface chemistry of the separated C-dots and the nature of the used mobile phases, providing a theoretical basis and experimental operability for C-dot separation. So, the proposed system possesses the capacity for adequately separating hydrophilic, amphiphilic, and lipophilic C-dots. The polyamide chromatography, due to its versatile and powerful separation performances, not only provides more thorough separation effects but also helps to correct our false perceptions from inadequate purified C-dots.
研究领域:
材料化学
·
分析化学
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产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2019
·
IF 5.155
Xiaolu Chen,Yadan Zhai,Xia Han,Honglai Liu,Ying Hu
Mussel-inspired surface modification has been received great attention due to the universal adhesive properties of catechols for fabrication of multifunctional coatings , especially for gluing hydrophilic polymers to fabricate underwater-superoleophobic materials utilizing in oil/water separation. Despite the extensive research carried out on this topic, the similarity and discrepancy between catecholamine and catecholic amino acid on surface modification and post functionalization have not been fully addressed yet. In this work, underwater superoleophobic surfaces have been successfully developed by a two-step dip-coating method with mussel-inspired coatings and subsequent zwitterionic sulfobetaine methacrylate (SBMA) grafting onto stainless steel meshes and used in oil/water separation. Here, dopamine and 3,4-dihydroxy-L-phenylalanine were both served as mussel-adhesives. More specifically, small molecule zwitterion rather than polyzwitterion was functionalized onto mussel-inspired coatings to minimize the effect of surface topography on surface wettability . The modified surfaces were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), and contact angle measurements to observe the surface morphology , estimate the surface roughness , and evaluate the wettability, respectively. It showed that SBMA modified meshes with polydopamine (PDA) or poly(3,4-dihydroxy-L-phenylalanine) (PDOPA) layer possessed quite different surface roughness, while both presented excellent oil repellency in water with underwater oil contact angles of 153°–160°, indicating a less dependence on surface roughness. Although by using the small molecule as the hydrophilic functionalized groups, the as-prepared meshes exhibited good self-cleaning and oil/water separation performance (separation efficiency >98% for hexane and >97% for soybean oil) and outstanding recyclability with 98% separation efficiency after 30 cycles. This method provides insight into different properties of polycatechols and simplifies the fabrication process through the use of small molecule zwitterion rather than zwitterionic polymer. Besides, the modified meshes also exhibited excellent stability for long-term use. The resulting underwater superoleophobicity and robust self-cleaning ability promise an ideal candidate for oil/water separation and oil contamination restriction.
研究领域:
材料科学
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表面工程
·
环境科学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Juan Yang,Xiang Liu,Kexin Song,Xinyue Li,Dihua Wang
Understanding of the correlation between physico-chemical property of adsorbent and the adsorption performance of contaminant is very significant for developing high-efficient materials to remove antibiotic contamination from water. In this work, a novel kind of carbon adsorbent (EC) derived from CO 2 and activated ECs with modified structure via a facile chemical method using H 2 and KOH were prepared. The synthetic carbon materials (EC, EC-H 2 , and EC-KOH) were then applied to remove tetracycline (TC). The kinetics of adsorption for these three carbon materials all well fitted the pseudo-second-order kinetic model. The experimental data of adsorption isotherm had good compatibility with Langmuir and Freundlich models (R 2 > 0.90), but the Temkin model was the most applicable for all adsorbents (R 2 > 0.98). A super-high adsorption capacity of EC-KOH obtained from Langmuir fitting was 933.56 mg g −1 , which was much higher than that of EC-H 2 (538.91 mg g −1 ) and EC (423.30 mg g −1 ), possibly due to its larger specific surface area (S BET ), pore volume, and specific surface chemical structure. Moreover, it was found that surface functional groups and large aperture of adsorbents had a positive effect on adsorption rate. More adsorption sites and surface functional groups of adsorbents were beneficial to enhance the adsorption affinity. These results are of great benefit to the directional control of carbon structure to increase the adsorption performance in rate, capacity, and affinity of antibiotics.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CARBON
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2018
·
IF 7.082
Dandan Han,Yucong Jiao,Wenqian Han,Guanhong Wu,Tongtao Li,Dong Yang,Angang Dong
Heteroatom doping of carbonaceous materials can effectively modulate their physiochemical properties, providing great potentials to design innovative architectures with enhanced performance for energy-related applications. Herein, we report a versatile molecular-based strategy for the in-situ synthesis of highly-ordered, heteroatom-doped mesoporous carbon frameworks (MCFs). Our approach is based on the transformation of self-assembled superlattices consisting of Fe 3 O 4 nanocrystals (NCs) with desired surface-coating molecular species, which are realized by exploiting versatile surface chemistry of colloidal NCs. By this strategy, various heteroatoms, such as N, B, and S, can be directly incorporated into the simultaneously formed MCFs with a homogeneous distribution . Taking advantage of their highly ordered and interconnected mesoporosity, tunable doping level, and high surface area, such heteroatom-doped MCFs show great promise for energy-related applications. We show that the N-doped MCFs (N-MCFs) exhibit significantly enhanced catalytic activity relative to their undoped counterparts when evaluated as electrocatalyst for oxygen reduction reaction . Likewise, the N-MCFs can also be used as electrode material for constructing supercapacitors with outstanding cycling stability and rate performance. This work offers a surface chemistry approach for the direct synthesis of highly-ordered MCFs containing homogeneously distributed heteroatoms, which are suitable for applications in various energy conversion and storage devices.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
JOURNAL OF CHROMATOGRAPHY A
·
2018
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IF 3.716
Yujie Zhang,Qiaoqi Li,Benlin Dai,Shouyong Zhou,Mingliang Zhang,Haifeng Han,Hongdeng Qiu
A new polar-embedded aromatic stationary phase has been prepared by covalently attaching p -biphenylacetamide silane to silica spheres. The retention behavior of this phase was compared with an alkylamide counterpart and octadecyl phases using different classes of analytes, including geometric isomers and congeners from Standard Reference Materials 869b, 870 and 1647e, positional isomers of electron-deficient benzenes, as well as alkylbenzenes and alkylbiphenyls. The relationship between shape selectivity and surface chemistry of stationary phase was comparatively studied. Influences of the embedded group and ligand length and/or size on the chromatographic selectivity towards various congeners were established. The new polar-embedded aromatic phase possessed unique benzenoid affinity, enhanced aromatic selectivity, distinct charge-transfer properties, as well as good water-wettablity, as a result it can be employed in normal phase, reversed-phase and per -aqueous modes.
研究领域:
分析化学
·
色谱技术
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产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 27
·15149-15157
·
IF 2.936
Wenhui Gao,Guangmei Zhai,Caifeng Zhang,Zhimeng Shao,Lulu Zheng,Yong Zhang,Yongzhen Yang,Xuemin Li,Xuguang Liu,Bingshe Xu
An initial improvement in performance of PbS quantum dot solar cells composed of one thick layer of PbS quantum dots (QDs) treated with tetrabutylammonium iodide (PbS–TBAI) and one thin layer of PbS QDs capped with 1,2-ethanedithiol (PbS–EDT) over short-term air exposure is widely observed. However, the underlying mechanisms still remain elusive. In the work, we sought to understand the mechanisms as well as their physicochemical origins using a combination of X-ray photoelectron spectroscopy (XPS) and various electronic measurements. It is found that the PbS–TBAI film plays a dominant role in the initial device performance improvement compared with the PbS–EDT film. The PbS–TBAI film is compensation doped upon short-term air exposure (one to three days) owing to the increase of Pb–O and/or Pb–OH species, enabling its energy band to align better with the electron transport layer for more efficient charge extraction. Moreover, it is demonstrated that the short-term air exposure is capable of reducing defects in the devices and improving the diode quality, resulting in an initial increase in device performance. This work contributes to the fundamental understanding of the surface chemistry changes of PbS quantum dots treated by different ligands over air-exposure and the role of surface chemistry of quantum dots in optimizing their photovoltaic performance.
研究领域:
材料科学
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光伏技术
·
物理化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Materials Science & Engineering C-Materials for Biological Applications
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2017
·
IF 4.164
Yanli Liu,Jiazhu Xu,Yan Zhou,Zhaoyang Ye,Wen-Song Tan
Cellular behaviors can be affected by both surface chemistry and topography of biomaterials substrates. The object of the present study was to investigate how pore structure and bioactive molecules regulate the adhesion and proliferation of rabbit bone marrow-derived mesenchymal stem cells (rMSCs) in synergy. Poly(ε-caprolactone) (PCL) films with a honeycomb-like porous structure were fabricated via a breath-figure method, and then further coated with bioactive molecules including four combinations of polyelectrolytes (GEL/CS, GEL/HA, CHI/CS and CHI/HA) via a layer-by-layer self-assembly (LBL) process. rMSCs were seeded on these films to evaluate both adhesion and proliferation. It was shown that a uniform honeycomb-like porous structure with a pore size of 18.87 ± 3.25 μm was obtained in the films. Bioactive molecules were proven to be successfully deposited on the films, the amount of which increased with the number of assembled layer. Both surface pore structure and assembled molecules play significant roles on the adhesion and proliferation of rMSCs. Notably, the spatial distribution of cells (either entrapped in pores or spreading over pores) on porous films was also dictated by the identity of the assembled molecules. These findings might be fundamental to design bioactive scaffolds for tissue engineering.
研究领域:
生物材料学
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组织工程学
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产品关联
DOI
PubMed
高影响因子
Materials Research Express
·
2020
·Vol. 7
·期 2
·025027
·
IF 1.929
Hong Zhao,Diandian Liu,Shujuan Xu,Yao Chen,Fujun Yin,Tao Yang,Mingyan Wang,Hua Deng,Wei Zhang,Weiwei Liu,Xiaohong Liu
Active electrocatalysts are the key to water splitting for hydrogen production through the electrolysis. In this paper, 50 nm silver nanoplates were used as templates for synthesis of Au–Ag island-shaped nanoplates by controlling the surface chemistry. The guiding mechanism of polyvinylpyrrolidone (PVP, Mw = 40 000) to Au–Ag island-shaped nanoplates crystal was also further investigated. It is found that the surface energy of Ag nanoplates between (100) and (111) crystal planes can be regulated by varying the amount of PVP in the system. Then a uniform Au-Ag triangular island nanostructure was obtained. Compared with the Ag nanoplates catalysts, the Au–Ag island nanoplates catalysts show the superior catalytic performances in hydrogen evolution electrocatalysis (HER). These results demonstrate a new surface chemistry modification by PVP and a galvanic displacement reaction for designing the active electrocatalysts. More importantly, the Au–Ag island-shaped nanoplates show an unconventional growth mode of preserving the original Ag nano-triangular crystal structure. The enhanced performance in electrocatalysis can be mainly attributed to Au–Ag alloy structure, which allows the appearance of synergistic effects. The present work demonstrates the crucial roles of surface chemistry in catalysts synthesis, which may guide the design of active bimetallic catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Siqi Gong,Fan Zhao,Huiting Xu,Meng Li,Junjie Qi,Honghai Wang,Zhiying Wang,Xiaobin Fan,Chunli Li,Jiapeng Liu
MXene has attracted a wide spread attention as promising supercapacitor electrode materials owing to excellent electronic conductivity and reversible surface redox capability. In fact, the supercapacitor performance strongly relies on surface terminations of MXene. However, regulating the types of surface terminations for enhancing the electrochemical performance of MXene is still one of major challenge. Herein, we successfully prepared a MXene containing iodine terminations (I-Ti 3 C 2 MXene) by facile Lewis-acidic-melt etching method and comprehensively investigated its supercapacitor performance. Benefiting from the presence of iodine terminations, the I-Ti 3 C 2 MXene with pseudocapacitor property exhibits significantly higher specific capacitance than that of hydrofluoric acid etching MXene (HF-Ti 3 C 2 T x MXene). Impressively, the I-Ti 3 C 2 MXene shows extraordinary long-term cyclic performance, even when cycled at high current density of 50 A/g, that the specific capacitance retention of 91% can be obtained over 100,000 cycles, corresponding to an average specific capacitance loss of only 0.00009% per cycle. Furthermore, the mechanisms involved were clarfied by systematical characterizations. This work will provide new insights for enhancing the supercapacitor performance of MXene-based materials by surface chemistry modification.
研究领域:
材料科学
·
电化学
·
储能技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nanoscale
·
2020
·Vol. 12
·期 32
·16987-16994
·
IF 6.895
Qian Sun,Jian Wang,Xiang Wang,Jie Dai,Xiaoshan Wang,Huacheng Fan,Zhiwei Wang,Hai Li,Xiao Huang,Wei Huang
MXenes, a rapidly developing family of two-dimensional materials possessing tunable electronic properties and abundant surface functional groups, are promising gas-sensing materials. Ti2CTx, with a thinner unit cell thickness compared to its compositional analogue Ti3C2Tx and thus more profound surface-dependent properties, has been less explored over the past years. Herein, by etching the precursor Ti2AlC with a concentrated HF or LiF/HCl mixture, semiconducting Ti2CTx (HF) nanosheets and metallic Ti2CTx (LiF/HCl) nanosheets were obtained, respectively, arising from their treatment-dependent surface functionalization. In addition, the resulting metallic nanosheets were partially oxidized into TiO2/Ti2CTx (LiF/HCl) hybrid, which exhibited superior sensitivity toward NH3 gas as compared with Ti2CTx (HF) and Ti2CTx (LiF/HCl). Detailed analysis suggests that a high concentration of surface oxygen containing species, such as –Ox, –(OH)x and Ti–O–Ti, is generally beneficial for NH3 sensing, and a relatively higher –Ox concentration allows rapid gas desorption and sensor recovery.
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）