Science China-Chemistry
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2023
·Vol. 66
·期 12
·3636-3644
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IF 9.6
Wang Shuangyue,Yang Ganceng,Jiao Yanqing,Liu Yue,Tian Chungui,Wu Aiping,Yan Haijing
Electrooxidation of the biomass derivative 5-hydroxymethylfurfural (HMF) is a highly promising approach for attaining versatile value-added chemicals ( e.g. , 2,5-furandicarboxylic acid, FDCA). Ni-based sulfides are promising electrocatalysts for HMF electrooxidation reaction (HMFOR). However, the HMFOR activity of Ni-based catalysts is far from satisfactory due to the unfavorable adsorption of HMF and OH*. Herein, we propose controlled W doping to effectively modify the electronic configuration of nanostructured Ni 3 S 2 to manipulate adsorption of HMF and OH*, for efficiently converting HMF into FDCA. Experimental and theoretical calculations indicate the incorporation of high-valence W results in the upshift of d-band center of Ni 3 S 2 , which facilitates the adsorption and dissociation of water to produce more OH*. Meanwhile, the high-valence W has strong electron-withdrawing ability and attracts electrons from Ni, leading to the elevated Ni valence, which is beneficial to optimizing the adsorption energy of HMF. Both concurrently contribute to the superb HMFOR performance. As a result, W 20 -Ni 3 S 2 @NF with optimal W dopant exhibits a low driving potential (1.34 V vs. RHE at 10 mA cm −2 ), accompanying with the 100% HMF conversion, 99.2% FDCA selectivity, and 97.3% Faraday efficiency. This work provides a design principle for HMFOR electrocatalysts by modulating the adsorption behaviors of HMF and OH* via rational electronic structure engineering.
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CELLULOSE
·
2023
·
IF 5.7
Tang Peixin,Si Yang,Song Xiyu,Sun Gang
Volatile carboxylic acids (VCAs) are intensively generated via bioengineering and widely used in food, textile, and cosmetic industries, but the efficient separation, collection, and regeneration of VCAs still face challenges. Here, we report a design and application of novel hierarchically porous structures built on bacterial cellulose nanofibrous membrane to effectively adsorb VCAs and to reveal the adsorptive status of the material at the same time. By in situ growing a triazine-based porous organic polymer on the nanofibers, the composite achieved integrated features of the co-existence of micro/meso/macropores, high specific surface area (255 m 2 /g), good flexibility, and selective affinity to VCAs, resulting in record-high adsorption capacities toward formic acid (815.36 mg/g) and acetic acid (754.21 mg/g). Moreover, the introduction of colorimetric probes onto the composite allows a visual indication of the adsorption-desorption process, i.e., the working status of the material, in real time. The successful fabrication of a bifunctional, hierarchical porous cellulose-based nanofibrous membrane could inspire the development of green adsorbents with improved efficacy and flexibility for gas capture and filtration. Graphical abstract
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RARE METALS
·
2023
·
IF 8.8
Zhang Chen-Chen,Wei Sheng,Sun Li-Xian,Ouyang Yi-Fang,Xu Fen,Chu Hai-Liang,Pan Hong-Ge,Chen Li-Xin,Xiao Xue-Zhang
Electrocatalytic water splitting coupled with sustainable energies is identified as an environmentally friendly and renewable strategy to generate high-quality hydrogen for the fuel cells. However, the main challenge is to develop high performance, low cost and chemically stable electrocatalysts to decline the energy barriers and enhance the sluggish kinetics of hydrogen evolution reaction (HER). Herein, a three-dimensional hierarchically ordered macroporous Ru-CoP@NC electrocatalyst (3DOM Ru-CoP@NC) derived from ordered macro-microporous metal–organic frameworks has been prepared using the precursor@template and double-solvent methods. The prepared 3DOM Ru-CoP@NC catalyst exhibits an overpotential of 15 mV ( j = 10 mA·cm −2 ) and a reaction Tafel slope of 38 mV·dec −1 in alkaline electrolyte, which are superior to commercial Pt@C catalyst. Additionally, the overpotential and reaction Tafel slope of this catalyst in acidic media are 45 mV and 50 mV·dec −1 , respectively. The outstanding HER activities of 3DOM Ru-CoP@NC catalysts are ascribed to the 3D highly interconnected-reticular nanospaces that can increase effective reaction active sites. The N doped carbon framework improves the electronic properties and conductivity. Moreover, the strong interaction of Ru and CoP nanoparticles also boosts the HER process. These results indicate that 3DOM Ru-CoP@NC catalysts with high catalytic activities have a broad application prospect in the future. Graphic abstract
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-14
·
IF 16.6
Yang Yuxuan,Zhao Xiaodan,Wang Shuang,Zhang Yanfeng,Yang Aiming,Cheng Yilong,Chen Xuesi
Osteoarthritis is a worldwide prevalent disease that imposes a significant socioeconomic burden on individuals and healthcare systems. Achieving cartilage regeneration in patients with osteoarthritis remains challenging clinically. In this work, we construct a multiple hydrogen-bond crosslinked hydrogel loaded with tannic acid and Kartogenin by polyaddition reaction as a cell-free scaffold for in vivo cartilage regeneration, which features ultra-durable mechanical properties and stage-dependent drug release behavior. We demonstrate that the hydrogel can withstand 28000 loading-unloading mechanical cycles and exhibits fast shape memory at body temperature (30 s) with the potential for minimally invasive surgery. We find that the hydrogel can also alleviate the inflammatory reaction and regulate oxidative stress in situ to establish a microenvironment conducive to healing. We show that the sequential release of tannic acid and Kartogenin can promote the migration of bone marrow mesenchymal stem cells into the hydrogel scaffold, followed by the induction of chondrocyte differentiation, thus leading to full-thickness cartilage regeneration in vivo. This work may provide a promising solution to address the problem of cartilage regeneration.
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POLYMER BULLETIN
·
2023
·
IF 3.2
Chen Zhengpeng,Li Jie,Guo Hongyun,Zhang Yongdong,Ma Mingzhong,Zhou Xing,Yao Wenhuan,Ma Hengchang,Lei Ziqiang,Lu Dedai
Transcatheter arterial embolization has been used clinically for the treatment of intermediate to advanced unresectable tumors, which is a complex procedure and may pose other risks. In order to achieve an efficient and simple therapeutic diagnostic method for tumors, this paper is based on the fact that the fluorescence properties of AIE fluorescent molecules are similar to those of pH-responsive polyamino acid materials undergoing a “sol–gel” phase transition in a tumor micro-acid environment, and two polyamino acid materials, PGTTC and PGCLTGCL, were linked with TPA derivatives of AIE fluorescent molecules to obtain catheter-free embolic agents, PGTTC-DCDPP-2TPA and PGCLTGCL-DCDPP-2TPA. In tumor fluorescence imaging experiments in tumor-bearing mice, both were enriched at the tumor 72 h after injection and that of the PGCLTGCL-DCDPP-2TPA was stronger, moreover, the tumor cells were suppressed and necrotic after 25 days. Therefore, this pH-responsive noninterventional embolization combination therapeutic diagnostic system has good prospects for application in the field of combined therapeutic diagnostic multifunctional platforms.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-11
·
IF 16.6
Ma Dingren,Lian Qiyu,Zhang Yexing,Huang Yajing,Guan Xinyi,Liang Qiwen,He Chun,Xia Dehua,Liu Shengwei,Yu Jiaguo
The structure-activity relationship in catalytic ozonation remains unclear, hindering the understanding of activity origins. Here, we report activity trends in catalytic ozonation using a series of single-atom catalysts with well-defined M 1 -N 3 C 1 (M: manganese, ferrum, cobalt, and nickel) active sites. The M 1 -N 3 C 1 units induce locally polarized M − C bonds to capture ozone molecules onto M atoms and serve as electron shuttles for catalytic ozonation, exhibiting excellent catalytic activities (at least 527 times higher than commercial manganese dioxide). The combined in situ characterization and theoretical calculations reveal single metal atom-dependent catalytic activity, with surface atomic oxygen reactivity identified as a descriptor for the structure-activity relationship in catalytic ozonation. Additionally, the dissociation barrier of surface peroxide species is proposed as a descriptor for the structure-activity relationship in ozone decomposition. These findings provide guidelines for designing high-performance catalytic ozonation catalysts and enhance the atomic-level mechanistic understanding of the integral control of ozone and methyl mercaptan.
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POLYMER BULLETIN
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2023
·
IF 3.2
Wang Juan,Shi Weihe,Xiang Shanglin,Huang Han,Jiang Wanyuan,Chen Shuangjun
UV debonding acrylate pressure-sensitive adhesives (UPSAs) are necessarily applied in the semiconductor industry. To establish a comprehensively understood method is important to detect their bonding and debonding behaviors. In this paper, rheological methods, including Three Interval Thixotropy tests (3ITT) and Tack test modes were used for characterizing series of UPSAs. Vinyl groups were successfully grafted onto the acrylate copolymer chains through isocyanate condensation reactions, which were characterized by nuclear magnetic resonance spectroscopy, Fourier transform infrared spectroscopy and gel permeation chromatography. From the maximum normal force in the Tack test modes, UPSAs after UV irradiation showed obvious debonding behaviors in short-time stress analysis. The recovery percentage of the storage modulus in 3ITT tests indicated that 0.6 wt% isocyanate curing agent made the UPSAs good resistance to deformation. Under the limit of 30 wt% pentaerythritol diacrylate (PETA), the rheological adhesion performance of UPSAs increases accordingly with the PETA content, which was also confirmed by 180° peel strength tests. From the microscope images of the wafer surfaces after peeling off the UPSA tapes, rheological characterization methods can help designing UPSAs with clean debonding properties.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 11
·1-15
·
IF 2.9
Wang Xiangbing,Li Xiaoxia,Sang Wutang,Peng Hui,Ma Guofu
A novel eco-friendly polyvinyl alcohol-straw biodegradable agricultural film is prepared by simple film coating methods to address the poor degradation problems of residual films and the environmental pollution caused by traditional non-degradable agricultural films. Hydrothermally activated wheat straw was added to polyvinyl alcohol (PVA) solution as a reinforcing material. The morphological, structural, mechanical properties, water resistance, and degradability are carefully investigated in this study. The results show that the composite film has 34.1% higher water resistance, 10.8 ~ 15.4 MPa fracture stress, and 115 ~ 304% fracture strain. It also has appropriate wettability, high thermal stability, water resistance, light transmission, and excellent degradability. The prepared films are inexpensive and eco-friendly. They can be produced on a large scale and applied in biodegradable films.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2023
·Vol. 21
·期 1
·1-20
·
IF 10.2
He Xuesong,Lin Fengjuan,Jia Runqing,Xia Yang,Liang Zhaoyuan,Xiao Xiangqian,Hu Qin,Deng Xiongwei,Li Qun,Sheng Wang
Background Abnormally regulated long non-coding RNAs (lncRNAs) functions in cancer emphasize their potential to serve as potential targets for cancer therapeutic intervention. LncRNA ASBEL has been identified as oncogene and an anti-sense transcript of tumor-suppressor gene of BTG3 in triple-negative breast cancer (TNBC). Results Herein, multicomponent self-assembled polyelectrolyte nanocomplexes (CANPs) based on the polyelectrolytes of bioactive hyaluronic acid (HA) and chitosan hydrochloride (CS) were designed and prepared for the collaborative modulation of oncogenic lncRNA ASBEL with antago3, an oligonucleotide antagonist targeting lncRNA ASBEL and hydrophobic curcumin (Cur) co-delivery for synergetic TNBC therapy. Antago3 and Cur co-incorporated CANPs were achieved via a one-step assembling strategy with the cooperation of noncovalent electrostatic interactions, hydrogen-bonding, and hydrophobic interactions. Moreover, the multicomponent assembled CANPs were ulteriorly decorated with a near-infrared fluorescence (NIRF) Cy-5.5 dye (FCANPs) for synchronous NIRF imaging and therapy monitoring performance. Resultantly, MDA-MB-231 cells proliferation, migration, and invasion were efficiently inhibited, and the highest apoptosis ratio was induced by FCANPs with coordination patterns. At the molecular level, effective regulation of lncRNA ASBEL/BTG3 and synchronous regulation of Bcl-2 and c-Met pathways could be observed. Conclusion As expected, systemic administration of FCANPs resulted in targeted and preferential accumulation of near-infrared fluorescence signal and Cur in the tumor tissue. More attractively, systemic FCANPs-mediated collaborative modulating lncRNA ASBEL/BTG3 and Cur co-delivery significantly suppressed the MDA-MB-231 xenograft tumor growth, inhibited metastasis and extended survival rate with negligible systemic toxicity. Our present study represented an effective approach to developing a promising theranostic platform for combating TNBC in a combined therapy pattern.
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Food and Bioprocess Technology
·
2023
·
IF 5.6
Liu Yikun,Liao Li,McClements David Julian,Chen Xing,Cao Mengmeng,Liang Ruihong,Zou Liqiang,Liu Wei
Vanilla is one of the most widely used flavors in the food and beverage industry; however, it is thermally unstable and volatile. In this study, microparticles consisting of ternary complexes of vanillin/γ-cyclodextrin/dextran (V/C/D) were prepared, in which vanillin served as a crosslink between the γ-cyclodextrin and dextran. One end of vanillin was inserted into the interior of γ-cyclodextrin through hydrophobic interactions and hydrogen bonding, while the other end was bound to dextran through hydrogen bonding. The encapsulation efficiency of vanillin in the microparticles increased from around 59 to 92% when the mass ratio of dextran in the complexes increased (V/C/D ratio ranging from 1:9:0 to 1:5:4). Moreover, the crystallization peak of vanillin disappeared in complexes with higher dextran contents. The dispersibility of vanillin in cold water (4 ℃) increased as the dextran content in the complexes increased, with the highest value being 15 mg/mL. Encapsulation of vanillin within the microparticles protected it from volatilization during storage, with more than 90% being retained after holding at 60 ℃ for a month, as well as increasing its resistance thermal processing. The release of vanillin during baking (200 ℃, 30 min) could be controlled by altering the composition of the microparticles. Our findings provide a novel strategy for improving the stability and controlling the release of aromas. Graphical Abstract
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JOURNAL OF MATERIALS SCIENCE
·
2023
·Vol. 58
·期 38
·15100-15115
·
IF 4.5
Zhu Yuying,Ling Xin,Dong Qian,Liu Qinglei,Wu Yu,Jin Qingjun,Zhang Wang
The development of advanced microwave absorbing materials with high absorption intensity and broad bandwidth is crucial for applications in electromagnetic interference shielding and stealth technology. In this study, we propose a novel hybrid material composed of porous magnetic nanospindle@poly(3,4-ethylenedioxythiophene) (PEDOT)/MXene (Fe@P/MX), designed to achieve superior microwave absorption performance through impedance matching and electromagnetic loss mechanisms. The conductive PEDOT and MXene, combined with magnetic nanospindles, enable impedance matching and promote dielectric loss, which ultimately enhances microwave absorption. Additionally, the hybrid material contains multiple interfaces that induce interface polarization and strong absorption of electromagnetic waves. Electromagnetic parameters of composites can be easily modulated by adjusting the content of PEDOT, thereby optimizing microwave absorption performance. The results demonstrate improved performance compared to existing materials, with the minimum reflection loss of − 60.6 dB at 17.0 GHz under the thickness of 1.6 mm. Besides, the effective absorption bandwidth extends to 5.4 GHz under the thickness of 1.9 mm. This core–shell hybrid material has significant potential for practical applications requiring efficient microwave absorption. Graphical abstract
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Sui Bowen,Zhu Youliang,Jiang Xuemei,Wang Yifan,Zhang Niboqia,Lu Zhongyuan,Yang Bai,Li Yunfeng
Assembly of nanoparticles into macroscopic materials with mechanical robustness, green processability, and recastable ability is an important and challenging task in materials science and nanotechnology. As an emerging nanoparticle with superior properties, macroscopic materials assembled from carbon dots will inherit their properties and further offer collective properties; however, macroscopic materials assembled from carbon dots solely remain unexplored. Here we report macroscopic films assembled from carbon dots modified by ureido pyrimidinone. These films show tunable fluorescence inherited from carbon dots. More importantly, these films exhibit collective properties including self-healing, re-castability, and superior mechanical properties, with Young’s modulus over 490 MPa and breaking strength over 30 MPa. The macroscopic films maintain original mechanical properties after several cycles of recasting. Through scratch healing and welding experiments, these films show good self-healing properties under mild conditions. Moreover, the molecular dynamics simulation reveals that the interplay of interparticle and intraparticle hydrogen bonding controls mechanical properties of macroscopic films. Notably, these films are processed into diverse shapes by an eco-friendly hydrosetting method. The methodology and results in this work shed light on the exploration of functional macroscopic materials assembled from nanoparticles and will accelerate innovative developments of nanomaterials in practical applications.
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