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NEW JOURNAL OF CHEMISTRY · 2017 ·Vol. 41 ·期 5 ·1953-1958 · IF 3.269

Robust urethane-bridged silica aerogels available for water-carved aerosculptures

Yulu Zhang,Jin Wang,Yong Wei,Xuetong Zhang

Molecular bridged silica aerogels have received extensive interest in recent years due to their easily controlled mechanical properties varying with different organosilane precursors, and without any further post-modification. In this work, a series of novel and robust molecular bridged silica aerogels were prepared by using a symmetrical urethane-bridged monomer, named N,N-bis(propyltriethoxysilyl)carbamide (bPTSCA), which was synthesized via a solvent-free exothermic reaction between 3-isocyanatopropyltriethoxysilane (IPTES) and 3-aminopropyltriethoxysilane (APTES) for several minutes at normal temperature and pressure. The influence of catalysts on the obtained gels and aerogels was studied in detail. It was found that NH4F aqueous solution showed the most effective catalysis capability, and the corresponding aerogels were intact with slight shrinkages. The mechanical strength of these aerogels could reach as high as 100 times more than that of the native silica aerogels (unbridged), and the strength could be easily adjusted from a rigid region to an elastic region simply by varying the sample density. Moreover, these aerogels possessed an interesting character of regional shrinking when encountering with water, which made it possible to fabricate artistic aerosculptures with water or other polar solvents as a graver.

研究领域: 材料科学 · 化学工程
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Advanced Membranes · 2022 · IF 0

Bio-inspired molecular bridge anchoring GO laminates onto PAN substrate for molecular separation

Ning Zhang,Hui Yu,Haoyu Cui,Hui Xiao,Xiaobin Jiang,Yan Dai,Xiaopeng Zhang,Junjiang Bao,Gaohong He

Graphene oxide (GO) films are highlighted to have great potential in water purification. The highly chemical and thermally stable polyacrylonitrile (PAN) competently constructs a superior substrate supporting the ultrathin GO laminates under various aqueous environments. However, the lack of available functional groups of PAN substrate, which inevitably leads to an undesirable water-induced peeling of the stacked GO laminates, greatly limits its practical application in constructing a stable GO composite membrane. A hydrolysis-condensation-induced bridge strategy is reported in which a bio-inspired molecular bridge generates a strong adhesion of PAN substrate to GO laminate, meanwhile interlaminar molecular bridges also form to generate a robust GO laminate with excellent resistance to swelling. Such GO composite membranes exhibit structural durability in the treatment of dye-containing wastewater for several days or even longer. The interfacial molecular bridge has little effect on the size-sieving and unique transport capability of the GO laminates. Comparable water permeability with the pristine GO laminates and nearly complete rejection to dyes (i.e. Congo red, methylene blue, and methyl orange) were obtained. The combination of easy fabrication, robust stability, and high performance make the PAN-supported GO membranes advantageous for practical application in textile wastewater purification.

研究领域: 材料科学 · 环境工程 · 化学工程
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ACS Applied Materials & Interfaces · 2023 · IF 9.5

Robust and Scalable In Vitro Surface Mineralization of Inert Polymers with a Rationally Designed Molecular Bridge

Mengxiao Zhang,Xiaohe Wang,Yunyun Xue,Jiaqi Li,Jianyu Wang,Chuanjie Fang,Liping Zhu

The artificial integration of inorganic materials onto polymers to create the analogues of natural biocomposites is an attractive field in materials science. However, due to significant diversity in the interfacial properties of two kinds of materials, advanced synthesis methods are quite complicated and the resultant materials are always vulnerable to external environments, which limits their application scenarios and makes them unsuitable for scalable production. Herein, we report a simple and universal approach to achieve robust and scalable surface mineralization of polymers using a rationally designed triple functional molecular bridge of fluorosilane, 3-[(perfluorohexyl sulfonyl) amino] propyltriethoxy silane (PFSS). In a two-step solution deposition, the fluoroalkyl and siloxane of the PFSS take charge of its adhesion and immobilization onto polymers by hydrophobic interaction and wrapping-like chemical cross-linking, and then the assembly and growth of inorganic nanoclusters for integration are achieved by strong chemical coordination of PFSS sulfonamide. The versatile mineralization of inorganic oxides (e.g., TiO2, SiO2, and Fe2O3) onto chemically inert polymer surfaces was realized very well. The resultant mineralized materials exhibit robust and multiple functionalities for hostile applications, such as hydrophilic membranes for removing oils in strong acidic and alkaline wastewaters, fabrics with advanced anti-bacteria for healthy wearing, and plates with strong mechanical performance for better use. Experimental results and theoretical calculations confirmed the homogenous distribution of the PFSS onto polymers via cross-linking for robust coordination with inorganic oxides. These results demonstrate a skillful enlightenment in the design of high-performance mineralized polymer materials used as membranes, fabrics, and medical devices.

研究领域: 材料科学 · 生物医学工程
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RSC Advances · 2015 ·Vol. 5 ·期 111 ·91407-91413 · IF 3.84

Autocatalytic synthesis of molecular-bridged silica aerogels with excellent absorption and super elasticity

Yong Wei,Jin Wang,Yulu Zhang,Lin Wang,Xuetong Zhang

In this study, molecular-bridged silica aerogels (MBSAs) were synthesized via supercritical CO2 liquid drying of bridged 3-aminopropyltriethoxysilane (APTES) wet gels, which were autocatalytic gelled by the catalyst-free bridging of APTES and 1,4-phthalaldehyde via a Schiff base condensation. The detailed mechanism of this facile, one-pot and autocatalytic approach for the production of MBSAs was revealed by in situ1H NMR and FTIR measurements, and the critical conditions for the successful autocatalytic gelation of the bridged-APTES were investigated. The densities and average pore diameters were in the range from 0.0535 to 0.0702 g cm−3 and from 12.9 to 14.1 nm, respectively. Moreover, the morphologies and thermal stability of the products were characterized by SEM and TGA, respectively. Interestingly, the MBSAs show excellent absorption performance for organic solvents, e.g., hexane, dichloromethane, kerosene, dimethylsulfoxide, tetrahydrofuran, ethanol, ethylsilicate, and N,N-dimethylformamide. Among those, 2437% by mass absorption of dichloromethane was achieved. Moreover, the absorption property of the aerogel was stable, with nearly no deterioration even after 30 absorption–desorption cycles. In addition, the aerogel showed remarkable flexibility, with the highest deformation of 90% and complete recovery after the release of stress, and it can be under through 30 cycles of compression–reversion process with 40% deformation.

CAS / MDL: 919-30-2 623-27-8
研究领域: 材料科学 · 化学工程
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PROGRESS IN ORGANIC COATINGS · 2025 · IF 7.3

Molecular bridge crosslinking and nano-ZnO synergistically construct fluorine/silicon-free multifunctional cotton fabric coatings

Chunyuan Jiang,Xinrui Zhang,Haizhen Ji,Jie Zhang,Xingjian Li,Shoufang Xu,Faqiang Li,Yinwen Li

Fluorine/silicon-free waterborne polyacrylate/nano-ZnO composite cotton fabric coatings (EPSAs) were developed to address the potential environmental and health risks posed by traditional fluorine-containing finishing agents. A molecular bridge constructed by 1,6-hexanediol diacrylate (HDDA) formed a crosslinked network, promoting synergistic directional alignment of tert-butyl and long-chain alkyl groups to create a low-surface-energy chemical hydrophobic barrier. Meanwhile, the polyvinyl alcohol (PVA) modified nano-ZnO not only improved the dispersibility of nano-ZnO, but also enhanced its mechanical stability through the hydrogen bonding interaction and interpenetrating network structure between PVA molecular chains and the polyacrylate main chains. Additionally, the PVA-modified nano-ZnO and polyacrylate jointly constructed a micro-nano rough structure on the fiber surface. This effectively inhibited water adsorption and enhanced impermeability. This hierarchical synergistic effect enabled the optimized EPSA 4 coating membrane to achieve 5.4 % water absorption over 7 d while the coated cotton fabric demonstrated a 128° water contact angle with 2.5 h effective water impermeability that remained stable after 50 washing cycles. Additionally, the coating significantly enhanced the cotton fabric's UPF value from 30.5 to 93.3 and achieved antimicrobial efficiencies of 99.98 % against Escherichia coli and 99.95 % against Staphylococcus aureus . By retaining their inherent breathability, this innovative coating system provided cotton fabrics with long-term hydrophobicity, antimicrobial functionality, and UV resistance, offering an environmentally sustainable multifunctional textile solution for applications including medical protective garments, outdoor technical textiles, and other sectors requiring integrated performance and eco-friendly characteristics.

研究领域: 材料科学 · 纺织工程 · 环境科学
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ADVANCED MATERIALS · 2024 · IF 27.4

Oriented Molecular Bridge Constructs Homogeneous Buried Interface for Perovskite Solar Cells with Efficiency Over 25.3%

Xinxin Wang,Hao Huang,Min Wang,Zhineng Lan,Peng Cui,Shuxian Du,Yingying Yang,Luyao Yan,Qiang Zhang,Shujie Qu,Meicheng Li

Buried interface optimization matters the efficiency improvement of planar perovskite solar cells (PSCs), and the molecular bridge is reported to be an effective approach. Herein, a molecular bridge is constructed at buried interface using 4-chloro-3-sulfamoylbenzoic acid (CSBA), and its preferred arrangement is systematically investigated. It is elucidated that the CSBA molecular is prone to be orientationally absorbed on TiO 2 surface through COOH–Ti, and then connect with perovskite through S═O–Pb, resulting in a feasible oriented molecular bridge. Contributing to the passivated interfacial defects, optimized interfacial energy level, and released perovskite tensile stress, resulting from the oriented CSBA molecular bridge, the PSCs with an active area of 0.08 cm 2 achieve a certified power conversion efficiency (PCE) of 25.32%, the highest among the TiO 2 -based planar PSCs. Encouragingly, the PSCs with an active area of 1 cm 2 achieve a champion PCE of 24.20%, significantly promoting the efficiency progress of large-area PSCs. In addition, the PSCs with oriented CSBA molecular bridge possess enhanced stability, the unencapsulated PSCs can maintain ≈91% and ≈85% of their initial PCE after 3000 h aging under ambient condition and 1200 h aging under exposure to UV irradiation.

CAS / MDL: 1205-30-7 7550-45-0
研究领域: 材料科学 · 能源科学
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Molecular bridges stabilize lithium metal anode and solid-state electrolyte interface

Chuankai Fu,Xu Zhang,Can Cui,Xueyan Zhang,Shuaifeng Lou,Yulin Ma,Hua Huo,Yunzhi Gao,Pengjian Zuo,Geping Yin

Rechargeable solid-state lithium metal battery (SSLMB) with high safety and energy density is regarded as one of the most promising candidates for next-generation energy-storage systems. However, the long-term interfacial stability between lithium metal anode and solid-state electrolyte is still a great challenge. Herein we propose an interfacial “molecular bridge” strategy to improve the interfacial adhesion between lithium metal anode and solid-state electrolyte by chemical bonding. As consequence, the lithium metal anode shows high interfacial wettability with solid-state electrolyte film, and Li/Li symmetrical cells display outstanding cycling stability with reduced polarization voltage, stable interfacial resistance, and dendrite-free lithium surface. In addition, high voltage LiCoO 2 (LCO)/Li full cells show enhanced cycling stability and superior rate capability. Moreover, the LCO/Li pouch cell exhibits excellent durability in harsh operating conditions such as bending and shearing. This scalable, simple and feasible interfacial-stabilization strategy offers a new route to the development and practical application of high-performance SSLMB.

研究领域: 材料科学 · 能源存储技术
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ELECTROCHIMICA ACTA · 2025 · IF 5.6

Novel organic molecular bridging strategy in Ti3CN interlayers towards stable and rapid sodium ions storage

Xiao-Rui Wang,Wen-Jie Shi,Ai-Jun Jiao,Zhen-Hai Fu,Min-Peng Li,Hong-Yan Li,Cai-Xia Zheng,Yu-Xia Hu,Hong-Tao Xue,Mao-Cheng Liu

MXenes is considered as one of the most potential sodium ions storage materials due to its superior metallic conductivity, abundant surface functional groups, extensive specific surface area, and tunable interlayer spacing. Nevertheless, its practical application is hindered by severe volumetric expansion/shrinkage and slow sodium ions diffusion during sodium ions insertion/extraction process. Herein, a novel organic acid molecules bridging strategy is reported to stabilize layered structure and adjust the interlayer spacing of Ti 3 CN, which is realized by bridging organic acid molecules (named as TOAA) into Ti 3 CN interlayers (named as Ti 3 CN-TOAA) to form strong amido (HN C=O) bonds. The carbonyl groups of TOAA molecules can not only provide active sites for sodium ions storage, but also inhibit volumetric expansion/shrinkage by providing strain/pillar effects within the Ti 3 CN interlayers, achieving stable and rapid sodium ions storage. Consequently, the interlayer spacing of Ti 3 CN-TOAA (1.42 nm) is enlargered compared with that of Ti 3 CN (1.22 nm), while the sodium ions migration barrier of Ti 3 CN-TOAA is reduced by 0.09 eV Ti 3 CN-TOAA demonstrates superior cycling stability (the capacity retention remains at 83.2% after 2000 cycles at 0.5 A g -1 ) and rate capability (2.5 times the capacity of pristine Ti 3 CN at 5.0 A g -1 ). Significantly, the Ti 3 CN-TOAA||AC sodium ions capacitor (SIC) exhibits excellent cycling stability, retaining 79.3% of its capacity after 8000 cycles at 1.0 A g -1 . This work presents a novel approach to achieving stable and rapid sodium ions storage by stabilizing layered structure and adjusting interlayer spacing.

研究领域: 材料科学 · 电化学
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 33 ·13997-14004 · IF 3.288

Core-template-free synthesis of molecularly ethane-bridged hollow mesoporous silica spheres from acid-hydrolyzed precursor

Yangyi Sun,Yijing Mao,Ningyu Di,Xiaolong Chen,Dongming Qi,Baoqing Shentu

Herein, using an acid-hydrolyzed tetraethyl orthosilicate (TEOS)/bis(triethoxysilyl)ethane (BTEE) mixture as a precursor for the traditional surfactant-assembly synthesis of mesostructured silica spheres instead of directly purchased commercial precursors, molecularly ethane-bridged hollow mesoporous silica spheres (MEB-HMSs) with radial mesochannels and an enlarged pore size were successfully synthesized without any additional core templates. The composition, pore size, particle size, shell thickness, and rate could be controllably tailored by only changing the amount of reagents used in the reaction. The cytotoxicity assay confirmed that MEB-HMSs have good biocompatibility, together with good Dox-loading capacity.

研究领域: 材料科学 · 生物医学工程
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CHINESE JOURNAL OF POLYMER SCIENCE · 2021 ·Vol. 39 ·期 11 ·1459-1469 · IF 3.603

Tuning the Johari-Goldstein β-Relaxation and Its Separation from α-Relaxation of Poly(n-alkyl methacrylate)s by Small Molecule-bridged Hydrogen Bonds

Liu Yuan-Biao,Shi Gao-Peng,Wu Guo-Zhang

Introducing small molecule-bridged hydrogen bonds (HBs) between polymer chains has been reported to effectively reduce the interchain cooperativity despite of strengthening the intermolecular interaction. Here, a systematic investigation on tuning the Johari-Goldstein β ( β JG ) relaxation by adding various low-molecular-weight phenols in poly( n -alkyl methacrylate)s is carried out to further clarify the anomalous dynamics. Given these small molecules capable of coupling the motion with pendent groups of host polymers due to forming at least two HBs per molecule, poly( n -alkyl methacrylate) mixtures exhibit rich dynamic changes in the β JG -properties and α, β JG separations. An increased loading of phenols with a small size and strong inter-HB strength (Δ υ i ) clearly benefits for significant retardation and suppression of the β JG -relaxation, narrows the α, β JG separation and converges the β JG -peak with the α -peak, which demonstrates the alleviation of inter-chain topological constraints. However, small molecules with a relatively big size and weak Δ υ i are found to amplify the magnitude of the α, β JG separation of poly(butyl methacrylate), even though experimental results of changes in α -dispersion and dynamic fragility confirm a reduction of the coupling factor n in all of these hybrids. The counterintuitive phenomenon suggests that the crossover time t c in the Coupling Model is no longer a universal quantity if the inter-chain interaction of polymers is strengthened by HBs. These compelling findings shed vital insights into the HB-induced anomalous dynamics, and provide essential guidance for tailoring the β JG behavior and designing glassy polymeric materials.

CAS / MDL: 2664-63-3
研究领域: 高分子化学 · 材料科学
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Nano Energy · 2024 · IF 16.8

PEDOT-molecular bridging foam-hydrogel based wearable triboelectric nanogenerator for energy harvesting and sensing

Shixia Lan,Yongyun Mao,Bingpu Zhou,Wanbiao Hu

Conductive hydrogels, due to their adjustable flexibility and conductivity, present considerable advantages in tackling the bottleneck issues associated with electron transfer in wearable electronic devices. However, during the deformation process, achieving effective electron transfer between the hydrogel electrode and the adjacent frictional piezoresistive sensing layer, as well as effective transmission within the hydrogel electrode itself, remains a significant challenge. Herein, PEDOT molecular bridging is proposed to establish an efficient connection between hydrogel electrode and the adjacent layer. Polyacrylamide integrated with PEDOT interpenetrating network-based hydrogel (PPNM) is prepared as electrode through synergistic dual-crosslinking. A repetitive vacuum-assisted dip-coating technique is employed to modify TPU foam scaffolds with silver nanowire (AgNW) and PPNM, resulting in TPU@AgNW@PPNM foam (TAP) with a three-dimensional dual-conductive network as the adjacent frictional piezoresistive sensing layer. By tightly integrating TAP with PPNM, a mutual PEDOT-bridging between TAP and PPNM is established. Importantly, the interface remains intact and ensures stable electron transmission even under significant stretching and bending conditions. The piezoresistive sensor and triboelectric nanogenerator assembled based on TAP and PPNM exhibited an enhanced sensitivity of 27.8 kPa −1 and an output power density of 3.1 mW m −2 , respectively. This innovative solution effectively addresses the critical issue of electronic transfer between the electrode layer and the adjacent layer in wearable electronic devices, while also mitigating the problems related to the rigidity of electrodes that can impact the flexibility and comfort of wearable devices.

研究领域: 材料科学 · 生物医学工程
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ADVANCED FUNCTIONAL MATERIALS · 2024 · IF 18.5

Coordination of Thermally Activated Delayed Fluorescent Molecules for Efficient and Stable Perovskite Light-Emitting Diodes

Bo Chen,He Liu,Jonghee Yang,Mahshid Ahmadi,Qi Chen,Ni Yin,Shitong Zhang,Meiqin Xiao,Haoyue Zhang,Long Xu,Ping Chen

The bandgap and operation stability of metal halide perovskites (MHPs) based light-emitting diodes (PeLEDs) have been compromised by the substantial surface defect densities in the matrix. Today's defect passivation strategies rely on coordination actions of small-molecular and/or polymeric ligands, which effectively enhance the optical properties of materials. However, the non-trivial insulating characteristics of the molecules concurrently sacrifice the operation stability and external quantum efficiency (EQE) of the PeLEDs by augmenting the charge injection barrier at the interface. Herein, a coordinative, charge-polarized organic semiconductor exhibiting thermally activated delayed fluorescence (TADF), namely 9,9-dimethyl-10-(4-(phenyl sulfonyl)phenyl)-9,10-dihydroacridine (SO-DMAc) is coordinated, into the MHPs matrix for deep-red PeLEDs. Owing to the distinctive charge transfer (CT) between the molecule and MHPs with exclusive coordination at the MHP's bottom, SO-DMAc serves as a molecular bridge that significantly augments the hole injection into the PeLEDs. Encouraged by these improvements, efficient and stable deep red PeLEDs offering EQE of 21.8% and respective half lifetimes (T 50 ) of luminance and EQE exceeding 6 and 35 h are demonstrated. It is revealed that the molecular coordination to the MHP surface is pivotal to manifesting the interfacial CT process for favorable energy level tuning.

研究领域: 材料科学 · 光电技术
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