Nature Catalysis
·
2021
·Vol. 4
·期 3
·202-211
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IF 41.813
Liu Hongfei,Xia Jun,Zhang Nan,Cheng Han,Bi Wentuan,Zu Xiaolong,Chu Wangsheng,Wu HengAn,Wu Changzheng,Xie Yi
Conventional strategies for modifying electrocatalysts for efficient CO 2 reduction are mainly based on doping, defect/morphology engineering, substrate design and so on. In most cases, these methods can only tune their structures, electronic states and thereby catalytic properties in a gradual way. Here we report that the solid–liquid phase transition of Ga–Sn/Ga–In alloys can induce an instant and radical transformation of their atomic and electronic structures during electrocatalysis, which dramatically impacts their catalytic properties. The transition of Sn/In active components from phase-segregated clusters to dispersed single atoms during melting results in a unique electronic structure through further reduction of both metallic Sn/In and Ga. Such atomic/electronic structure transitions can correlate well with suppression of the hydrogen evolution reaction and an enhanced formate Faradaic efficiency from <35% to >95%. This two-state switching strategy may be extended to other catalytic reactions to determine correlations between their structures and catalytic properties.
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MICROCHIMICA ACTA
·
2021
·Vol. 188
·期 4
·1-10
·
IF 5.833
Liu Wendong,Guo Junnan,Chen Chuanxia,Ni Pengjuan,Jiang Yuanyuan,Zhang Chenghui,Wang Bo,Lu Yizhong
Enzyme-mimetic properties of nanomaterials can be efficiently tuned by controlling their size, composition, and structure. Here, ultrathin PdCu alloy nanosheet–assembled three-dimensional (3D) nanoflowers (Pd 1 Cu x NAFs) with tunable surface composition are obtained via a generalized strategy. In presence of H 2 O 2 , the as-synthesized Pd 1 Cu x NAFs can catalyze the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) to the oxidized form of TMB (oxTMB) with a characteristic absorption peak at 652 nm. Interestingly, Pd 1 Cu x NAFs show obviously composition-dependent peroxidase-like catalytic activities because of the synergistic interaction of nanoalloy. Additionally, different from 2D Pd nanosheets, the distinctive 3D superstructures are featured with rich approachable sites and proper layer spacing, which are in favor of fast mass transport and electron transfers during the catalytic process. Among the studied Pd 1 Cu x NAFs, the Pd 1 Cu 1.7 NAFs show the highest enzyme-like activities and can be successfully applied for the colorimetric detection of glucose with a low detection limit of 2.93 ± 0.53 μM. This work provides an efficient avenue to fabricate PdCu NAF nanozymes in biosensing toward glucose detection. Graphical abstract
Two-dimensional (2D) PdCu ultrathin nanosheet–assembled 3D nanoflowers (Pd 1 Cu x NAFs) with tunable surface composition exhibit substantially enhanced intrinsic peroxidase-like catalytic activities. The Pd 1 Cu 1.7 NAFs are successfully used as peroxidase mimic catalyst for the colorimetric detection of glucose with low detection limit of 2.93 μM.
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JOURNAL OF ELECTRONIC MATERIALS
·
2021
·Vol. 50
·期 5
·2831-2839
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IF 1.938
Nie Jiajin,Li Zhitong,Shi Guifei,Wang Jing,Yao Shaowei
Fe-zeolitic imidazolate framework (ZIF)@C (Fe-ZIF wrapped by carbon) anode material has been manufactured. It has porous nanostructure, which can effectively shorten the distance of lithium ion transmission, thus achieving excellent rate performance, and can also reduce the volume expansion in the charging and discharging process, thus reducing the attenuation of capacity. The external carbon coating avoids direct contact between Fe-ZIF and the electrolyte, inhibits decomposition of the electrolyte, and impedes formation of the solid electrolyte interphase (SEI) film, thus obtaining higher reversible capacity in the cycling process. At a current density of 100 mA/g, Fe-ZIF@C achieves a high discharge capacity of 719 mAh/g after 100 cycles. This research shows that Fe-ZIF@C has potential for use as an anode material for lithium-ion batteries.
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FIBERS AND POLYMERS
·
2021
·Vol. 22
·期 12
·3510-3516
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IF 2.153
Chen Jiayi,Wang Kuang,Qi Zhenming,Wang Chunxia
BiVO 4 was prepared by Bi(NO 3 ) 3 ·5H 2 O and NH 4 VO 3 via a facial method. (3-acrylamide propyl) trimethyl ammonium chloride (ATAC) and allyl glycidyl ether (AGE) were reacted with 3-mercaptopropyl triethoxysilane (KH590) under ultraviolet irradiation, respectively, to prepare hydrophilic and reactive components. Then self-dispersive and reactive BiVO 4 nanoparticles were acquired after mixing hydrophilic and reactive components. Cotton fabric loaded with self-dispersive and reactive BiVO 4 was obtained by dipping-drying-curing method. BiVO 4 before and after modification was characterized by scanning electron microscope (SEM), Fourier transform infrared spectroscopy (FT-IR), zeta potential and particle size. X-ray diffraction (XRD), SEM and energy dispersive spectrum (EDS) were adopted to characterize crystal structure, surface morphology and chemical element components of cotton fabric. Ultraviolet protection and self-cleaning performance were investigated. Results showed that the dispersion stability of modified BiVO 4 was improved, and cotton fabric loaded with modified BiVO 4 possessed commendable ultraviolet protection and self-cleaning activities. The modified BiVO 4 with mole ratio of ATAC and AGE at 3:2 had the optimized dispersion stability, and the cotton fabric loaded with it featured the best ultraviolet protection and self-cleaning properties. The possible mechanism and reactions for the binding of BiVO 4 with cotton fabrics was proposed.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 21
·5409-5417
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IF 4.157
Han Shuang,Yao Aixin,Ding Yuxin,Leng Qiuxue,Teng Fu
In this study, a novel kind of imprinted polymers based on metal–organic frameworks (MOF@DES-MIPs) was prepared, using bovine hemoglobin (BHb) as template molecules and deep eutectic solvents (DES) as functional monomers for selective recognition and adsorption of BHb. MOF were used as the substrates to improve the accessibility of imprinted sites and DES as the functional monomers to produce different forces for BHb to help the formation of imprinted sites. Imprinted polymer films were taken to provide analyte selectivity. The MOF@DES-MIPs prepared were characterized and evaluated by scanning electron microscope, X-ray diffraction, and Fourier transform infrared spectrometer. We also investigated the influences of BHb concentration and adsorption time on the performance of MOF@DES-MIPs. The maximal adsorption capacity of MOF@DES-MIPs to BHb reached 151.28 mg g −1 , and the MOF@DES-MIPs showed good selectivity and fast adsorption equilibrium, which might offer a novel method for the preparation and research of molecularly imprinted polymers of biomacromolecules. In addition, MOF@DES-MIPs were successfully applied in the selective recognition of BHb from a real bovine blood sample.
Graphical abstract
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
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2021
·Vol. 32
·期 14
·18591-18604
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IF 2.478
Zhang Shengsheng,Huang Fanglin,Zhong Mingqiang,Fan Ping
Dielectric material is an important material for film capacitors. However, the progress of this material is either impeded by its low dielectric constant, high loss tangent, or insufficient flexibility. In this work, PVA/GO film with alternating layer structure was fabricated by Spin-Coating-Assembly (SCA) method. This alternating layer structure not only benefits forming numerous microscale capacitors which improve ε value a lot, but also helps eliminate perpendicular contact of GO and prevents the formation of conductive pathways. Thus, compared with pure PVA, significantly increased dielectric permittivity and a low loss tangent were simultaneously observed for the PVA/GO film. The ratio of dielectric permittivity to loss tangent increased from 68 to 165. These films might be potential flexible dielectric materials for advanced electrical devices such as embedded capacitors.
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Stem Cell Research & Therapy
·
2021
·Vol. 12
·期 1
·1-16
·
IF 6.832
Zhang Xinxin,Jiang Xiaorui,Jiang Shan,Cai Xiyu,Yu Shengji,Pei Guoxian
Background Tissue-engineered bone grafts (TEBGs) that undergo vascularization and neurotization evolve into functioning bone tissue. Previously, we verified that implanting sensory nerve tracts into TEBGs promoted osteogenesis. However, the precise mechanisms and interaction between seed cells were not explored. In this study, we hypothesized that neurotization may influence the osteogenesis of TEBGs through vascularization. Methods We cultured rat Schwann cells (SCs), aortic endothelial cells (AECs), and bone marrow-derived mesenchymal stem cells (BM-MSCs) and then obtained BM-MSC-derived induced endothelial cells (IECs) and induced osteoblasts (IOBs). IECs and AECs were cultured in an SC-conditioned medium (SC-CM) to assess proliferation, migration, capillary-like tube formation, and angiogenesis, and the vascular endothelial growth factor (VEGF) levels in the supernatants were detected. We established an indirect coculture model to detect the expression of nestin and VEGF receptors in IECs and tissue inhibitor of metalloproteinase (TIMP)-2 in SCs. Then, SCs, IECs, and IOBs were labeled and loaded into a β-tricalcium phosphate scaffold to induce prevascularization, and the scaffold was implanted into a 6-mm-long defect of rat femurs. Three groups were set up according to the loaded cells: I, SCs, and IECs (coculture for 3 days) plus IOBs; II, IECs (culture for 3 days) plus IOBs; III, IOBs. Nestin and TIMP-2 expression and osteogenesis of TEBGs were evaluated at 12 weeks post-implantation through histological and radiological assessments. Results We found that SC-CM promoted IEC proliferation, migration, capillary-like tube formation, and angiogenesis, but no similar effects were observed for AECs. IECs expressed nestin extensively, while AECs barely expressed nestin, and SC-CM promoted the VEGF secretion of IECs. In the coculture model, SCs promoted nestin and VEGF receptor expression in IECs, and IECs inhibited TIMP-2 expression in SCs. The promotion of prevascularized TEBGs by SCs and IECs in group I augmented new bone formation at 6 and 12 weeks. Nestin expression was higher in group I than in the other groups, while TIMP-2 expression was lower at 12 weeks. Conclusions This study demonstrated that SCs can promote TEBG osteogenesis via IECs and further revealed the related specific characteristics of IECs, providing preliminary cytological evidence for neurotization of TEBGs.
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ANALYTICAL AND BIOANALYTICAL CHEMISTRY
·
2021
·Vol. 413
·期 19
·4775-4784
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IF 4.157
Gao Ningning,Wang Qing,Tang Jun,Yao Shengyuan,Li Hongmei,Yue Xiaxia,Fu Jihong,Zhong Furu,Wang Tao,Wang Jing
Surface-enhanced Raman scattering (SERS), as a rapid, reliable and non-destructive spectral detection technology, has made a series of breakthrough achievements in screening and pre-diagnosis of various cancerous tumors. In this paper, high-performance gold nanoparticles/785 porous silicon photonic crystals (Au NPs/785 PSi PhCs) active SERS substrates were specially designed for serum testing, and realized highly sensitive detection of serum from healthy people, patients with cervical cancer and breast cancer. Based on the SERS spectra of the three groups of serum, the significant differences between the healthy group and cancer group at 1030 cm −1 and 1051 cm −1 were analyzed, and the similar but different serum SERS spectra of cervical cancer and breast cancer patients were compared. In addition, the spectral difference detected by SERS technology combined with a multivariate statistical algorithm was used to distinguish three kinds of serum. The serum SERS spectral sensitive bands were extracted by recursive weighted partial least squares (rPLS), and the three classification diagnosis models were established by combining orthogonal partial least squares discriminant analysis (OPLS-DA), linear discriminant analysis (LDA) and principal component analysis support vector machine (PCA-SVM) for synchronous classification and discrimination of the three groups of serum. The diagnostic results showed that the overall screening accuracy of three models were 93.28%, 97.77% and 94.78%, respectively. These above results confirmed that the Au NPs/785 PSi PhCs can realize super-sensitive detection of serum, and the established diagnostic model has great potential for pre-diagnosis and simultaneous screening of cervical cancer and breast cancer. Graphical abstract
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JOURNAL OF POLYMER RESEARCH
·
2021
·Vol. 28
·期 6
·1-11
·
IF 3.097
Wang Wei-Yu,Zha Xiang-Jun,Bao Rui-Ying,Ke Kai,Liu Zheng-Ying,Yang Ming-Bo,Yang Wei
Dynamics of exchange within vitrimer networks are influenced by mobility of the chemical species involved in the exchange reaction, then it can be affected by the crystalline phase when boronic ester bond is introduced into the thermoplastic elastomers with crystalline phase as physical cross-links. In this work, the dynamic dioxaborolane cross-links were introduced into commercial poly(ethylene-α-octene) (POE) with crystalline phases as physical cross-links to prepare POE vitrimers. The results of stress relaxation show that relaxation time (τ) follows an Arrhenius law with the temperature at the melting range for not only POE vitrimers and thermally treated POE vitrimers with dynamic cross-links, but also neat POE with purely physical cross-links. The liquid-to-solid transition temperature can raise to 35.3 °C for POE vitrimers from -42.9 °C of the thermally treated one, due to the constrained mobility by residual crystalline phases. The resulted POE vitrimers maintain a stress at break of higher than 27.5 MPa and an elongation at break of higher than 800% at room temperature. With the temperature increasing, the crystal melting induced weakening of the physical cross-linking in POE decreases the strength, but the storage modulus and the stress at 300% and 500% elongation of POE vitrimers are improved. The properties of POE vitrimers can almost keep unchanged after recycling or healing. All these results show that the introduction of reversible boronic ester bonds is a promising strategy to improve the performances and recyclability of physically cross-linked POE materials.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 19
·11426-11435
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IF 4.22
Yan Dong,Peng Zhen,Wang Wei,Zeng Peng,Huang Yiyin
Abstract Carbon-based metal-free catalysts exhibit great applications in electrochemical CO 2 reduction (ECR), while most studies merely focus on large-sized carbons with limited ratio of surface atoms for engineering to create surface active centers. Here, we report a joint treatment of C60 by heating and plasma to induce a dramatic performance promotion during ECR. The electrochemical measurements indicate the Faraday efficiency for ECR toward CO production kept at high level over 80% in a wide potential region from − 0.4 to − 0.7 V versus RHE, with the highest value reaching 96.8%. The physical characterization reveals that fragmentation of C60 occurs together with N/O doping, both of which could induce change in electron structure, causing the formation of *COOH intermediate and ultimately leading to the optimized activity and selectivity for CO production. This treatment route was further revealed to be applicative for other carbon materials, e.g., single-walled carbon nanotube, to promote its ECR activity and selectivity. Graphical Abstract
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 8
·10951-10962
·
IF 2.478
Zhang Yakang,Liang Xuan,Jiang Mengting,Liang Qian,Xu Song,Yao Chao,Zhou Man,Li Zhongyu
Based on the three-dimensional ordered macroporous titanium dioxide (3DOM-TiO 2 ), a series of gold-embedded 3DOM-TiO 2 ( n Au@3DOM-TiO 2 ) with controlled Au loading amount ( n = 0.24, 1.2, 2.4, 4.8, 12, and 24 wt%) was successfully fabricated via in-situ pyrolysis for the first time. Compared with the surface-modified Au/3DOM-TiO 2 by traditional impregnation–reduction route, this body-doped Au@3DOM-TiO 2 structure exhibited smaller particle size and better dispersive property which are important for photocatalysis. Therefore, the photocatalytic activities of n Au@3DOM-TiO 2 have been tested and the optimized photocatalyst of 4.8Au@3DOM-TiO 2 was identified. A possible mechanism of Au@3DOM-TiO 2 for the enhanced photoactivity was well discussed. The present work demonstrated a unique “gold-embedded” interface with potential advantages of highly dispersed, anti-aggregation, easy recovery, and enhanced catalytic performance, and that this approach could provide an ideal platform for the further design of noble metal-doped semiconductors.
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JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 19
·11266-11277
·
IF 4.22
Zeng Qingtao,Ma Piming,Lai Dehui,Lai Xuejun,Zeng Xingrong,Li Hongqiang
Abstract In recent years, eco-friendly superhydrophobic materials have aroused much attention. Herein, biodegradable poly(lactic acid) (PLA) was selected as basic material to fabricate superhydrophobic foam with electrothermal effect by dip-coating graphene oxide (GO) on the surface of PLA foam constructed through freeze-drying process and the subsequent reduction with hydroiodic acid. Owing to the micro-nano rough structure of pristine PLA foam and the coverage of low-surface-energy reduced GO (rGO), the obtained rGO@PLA foam exhibited excellent water repellency with a high water contact angle of 150.6°. The foam was able to separate different oil–water mixtures, and the separation efficiencies were all above 96%. Importantly, the rGO layer also endowed the PLA foam with electrothermal conversion capability, and the surface temperature of the rGO@PLA foam rapidly increased to 129.5 °C from 30.8 °C at a low voltage of 15 V within only 120 s. By means of the generated Joule heat, the rGO@PLA foam was successfully applied for separating viscous crude oil from water, and the separation rate was about 14 times higher than that without voltage. Our findings conceivably stand out as a new tool to fabricate functional biodegradable materials for clean-up of viscous crude oil. Graphical abstract
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危险品化学品经营许可证（带存储）