INORGANIC CHEMISTRY
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2023
·
IF 4.6
Lan Ding,Yongping Ding,Fenghua Bai,Gonglai Chen,Shuwei Zhang,Xiaoxue Yang,Huiqin Li,Xiaojing Wang
Given the global warming caused by excess CO2 accumulation in the atmosphere, it is essential to reduce CO2 by capturing and converting it to chemical feedstock using solar energy. Herein, a novel Cs3Bi2Br9/bismuth-based metal–organic framework (Bi-MOF) composite was prepared via an in situ growth strategy of Cs3Bi2Br9 quantum dots (QDs) on the surface of Bi-MOF nanosheets through coshared bismuth atoms. The prepared Cs3Bi2Br9/Bi-MOF exhibits bifunctional merits for both the high capture and effective conversion of CO2, among which the optimized 3Cs3Bi2Br9/Bi-MOF sample shows a CO2–CO conversion yield as high as 572.24 μmol g–1 h–1 under the irradiation of a 300 W Xe lamp. In addition, the composite shows good stability after five recycles in humid air, and the CO2 photoreduction efficiency does not decrease significantly. The mechanistic investigation uncovers that the intimate atomic-level contact between Cs3Bi2Br9 and Bi-MOF via the coshared atoms not only improves the dispersion of Cs3Bi2Br9 QDs over Bi-MOF nanosheets but also accelerates interfacial charge transfer by forming a strong bonding linkage, which endows it with the best performance of CO2 photoreduction. Our new finding of bismuth-based metal–organic framework/lead-free halide perovskite by cosharing atoms opens a new avenue for a novel preparation strategy of the heterojunction with atomic-level contact and potential applications in capture and photocatalytic conversion of CO2.
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高影响因子
JOURNAL OF MOLECULAR LIQUIDS
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2023
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IF 6
Ding Jiang,Yuting He,Jinrui Zhang,Jie Yin,Jing Ding,Shuang Wang,Hongping Li
Conjugate acid-base bi-functional PILs (CAB-PILs) with carboxylate and carboxyl branches were synthesized and used as catalysts for the cycloaddition reaction of glycidol with CO 2 . Two functional ionic monomers, 3-(carboxymethyl)-1-vinyl-1H-imidazol-3-ium chloride (CEImCl) and 2-(1-vinyl-1H-imidazol-3-ium-3-yl) acetate (CCIm), were introduced into the CAB-PILs skeleton. In this case, we proved the excellent characteristics of the catalyst containing both Lewis base and Bronsted acid sites for converting CO 2 to cyclic carbonate under mild conditions. The catalyst showed good reusability and remained excellent activity after five reaction cycles. Combined with XPS, FTIR and DFT calculations, it is proved that the CCIm ionic monomer not only play the role of CO 2 absorption center, but also has synergistic effect with CEImCl in CAB-PILs to promote cycloaddition reaction.
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Applied Materials Today
·
2022
·
IF 8.663
Shaohua Wu,Wenwen Zhao,Mingchao Sun,Peng He,Hongyu Lv,Qiuyu Wang,Shuo Zhang,Qian Wu,Peixue Ling,Shaojuan Chen,Jianwei Ma
The clinical treatment of chronic wounds caused by different pathophysiological ulcers like diabetic ulcers still remains a bottleneck. Although numerous approaches have been designed and developed, their therapeutic effects cannot meet the medical needs due to the complicated pathological microenvironment and restricted regenerative capacity of hard-healing chronic wounds. In this study, novel bi-layered and multifunctional dressing patches constructed with one layer of electrospun methacrylated gelatin (MeGel)/poly (L-lactic acid) (PLLA) radially-oriented nanofiber mats (RNMs) and one layer of Salvia miltiorrhiza Bunge-Radix Puerariae herbal compound (SRHC)-loaded MeGel hydrogel were designed to promote the closure and healing of diabetic wounds. An innovative electrospinning method was firstly designed and implemented to generate MeGel/PLLA RNMs, which were demonstrated to be a more appropriate nanofiber pattern for effectively guiding migration and promoting proliferation of human dermal fibroblasts (HDFs) compared with the conventional electrospun MeGel/PLLA haphazardly-oriented nanofiber mats (HNMs) and MeGel/PLLA uniaxially-oriented nanofiber mats (UNMs). Importantly, the in vivo mice acute full-thickness defect models also confirmed that MeGel/PLLA RNMs could significantly promote the cell migration and accelerate the healing rate throughout providing the cell recruitment and regulation abilities in comparison with MeGel/PLLA HNMs and UNMs. The MeGel hydrogel precursors loaded with different concentrations of SRHC were employed to generate the hydrogel layers on the MeGel/PLLA RNMs, and therefore a series of bi-layered wound dressing patches with integrated multifunctional properties were fabricated. All the bi-layered wound dressing patches with or without SRHC showed excellent hemostatic performances. The bi-layered dressing patches containing SRHC exhibited great antibacterial property to both E. coli and S. aureus , and also high cell survival rate to HDFs. For the in vivo full-thickness diabetic wound healing test, the bi-layered dressing patches without SRHC exhibited a faster wound healing rate compared with the medical gauzes. Furthermore, the 10% SRHC loaded bi-layered dressing patches significantly accelerated the high-quality regeneration and healing of diabetic wounds by effectively reducing the inflammation, promoting the vascularization, and facilitating the regeneration of hair follicles. Specifically, the 10% SRHC loaded bi-layered dressing patches presented a high healing area of 97.4 ± 2.8% at day 18 after surgery. Our present study demonstrated that the SRHC contained bi-layered dressing patches show great potential for the treatment of hard-healing diabetic wounds.
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Journal of Cleaner Production
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2022
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IF 11.072
Junfeng Miao,Zuozhao Zhai,Shasha Wang,Yuelong Xu,Shichao Du,Xiaolei Wang,Xiaoxi Dong,Bin Ren,Zhenfa Liu
The hierarchical porous nitrogen-doped two-dimensional carbon (HNGC) was prepared by simple calcination of magnesium sulfate (MgSO 4 ) and self-synthesized nitrogen-doped two-dimensional graphene-like carbon at a mild temperature in oxygen. The influence MgSO4 on the morphology, structure and chemical composition of the prepared HNGC samples were studied using scanning electron microscopy, transmission electron microscopy , X-ray diffraction, Raman spectroscopy , surface area analysis, X-ray photoelectron microscopy and elemental analyzer. HNGC-2 exhibited a uniform three-dimensional coral-like porous inter-connected structure, large specific surface area, high pore volume, and no loss of nitrogen content. HNGC-2 demonstrated an excellent rate capability of 62.8% at 20 A g −1 , outstanding stability of 96.1% following 5000 cycles and the assembled symmetric supercapcitor achieved 12.5 Wh kg −1 at a 350 Wkg -1 and 7.5 Wh kg −1 at 3500 Wkg -1 . The novel method was also found to be effective for facilitating the electrochemical performance of commercial biomass active carbon. In addition, HNGC-2 was used for the photo-catalytic degradation of methylene blue and over 99% of methylene blue was successfully degraded under 25-min visible irradiation in the presence of potassium persulfate. The enhanced electrochemical performance and the excellent photo-catalytic performance of HNGC-2 indicated that porous carbon can be successfully activated using an appropriate oxidation strategy.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Weihua Qin,Mingye Ren,Yuwei Lu,Shaoxia Yang
The two-stage fixed-bed reactor significantly enhanced the phenol degradation efficiency in the heterogeneous Fenton-like reaction. The Cu/Bi-Ce/Al 2 O 3 catalyst, prepared by impregnation-precipitation method, exhibited favorable phenol removal, and the phenol degradation efficiency was ∼32.6 % higher in the two-stage fixed-bed reactor than that in the one-stage fixed-bed reactor under optimal parameters. Moreover, the Cu/Bi-Ce/Al 2 O 3 catalyst had excellent stability in the Fenton-like reaction due to the bismuth doping in the catalyst inhibiting the dissolution of copper ion. The Cu/Bi-Ce/Al 2 O 3 catalyst also displayed efficient purification ability for phenolic municipal sewage in the two-stage fixed-bed reactor. The redox cycles of Cu 2+ /Cu + and Ce 4+ /Ce 3+ were evidenced coexist to enhance the catalyst activity. The quenching experiments demonstrated that the generated singlet oxygen and superoxide anion free radicals dominated the degradation of phenol in the heterogeneous Fenton-like reaction over the Cu/Bi-Ce/Al 2 O 3 catalyst. This study may provide a novel heterogeneous Fenton-like/H 2 O 2 system for degrading organic pollutants in the fixed-bed reactor.
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Processes
·
2021
·Vol. 9
·期 9
·1487
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IF 2.847
Muhammad Faizan,Kifayat Ullah Khan Niazi,Hasnain Nawaz,Niaz Muhammad,Hao Li,Fei Dai,Ruirui Zhang,Ruixia Liu,Suojiang Zhang
In recent work, deep eutectic solvents (DESs) as ionic liquid analogues have been abundantly used in catalysis. Herein, vanadium phosphorus oxide (VPO) catalysts were synthesized from mono-, bi-, and tri- metallic DES of Nb, Zr, and Mo metal dopants as structure-directing agents and electronic promoters for n-butane selective oxidation towards maleic anhydride. Higher MA selectivity and larger n-butane conversion was successfully obtained using the newly developed catalysts, while oxidation by-product COx(CO, CO2) was minimized. Characterization techniques including FTIR, DSC, XRD, TEM, SEM, EDS, Raman spectroscopy, TGA, XPS, and NH3-TPD were employed to fully characterize the DESs, precursors and catalysts. This work led to an increase of 7.8% in MA mass yield with 16% more n-butane conversion as compared to an unpromoted VPO catalyst. Moreover, the utilization of a low-carbon alkane brought in a green impact on the chemical plant as well as the environment.Keywords:deep eutectic solvent;vanadium phosphorus oxide;n-butane selective oxidation;structure directing agent;electronic promoter
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ACS Applied Nano Materials
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2021
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IF 5.097
Qian Wang,Huanshun Yin,Jia Ding,Yunlei Zhou,Shiyun Ai
5-Formyluracil (5fU) is considered an important epigenetic modification agent involved in gene regulation, cell differentiation, and development. 5fU exists in many cells and tissues but is highly similar to the structure of 5-formylcytosine (5fC) and is less abundant in genome. Therefore, the development of a rapid, sensitive, and highly selective method to detect 5fU is desired. In this study, a photoelectrochemical biosensor based on WS2/Bi/BiOBr nanocomposites, black TiO2 (b-TiO2), and hemin/G-quadruplex was described, which was found to be highly sensitive and selective for 5-formyluracil-2′-deoxyuridine-5′-triphosphate (5fdUTP) detection. WS2/Bi/BiOBr was first employed as a photosensitive material, and 3,4-diaminobenzoic acid (DABA) was adopted as a 5fdUTP recognition and capture reagent, where DABA was captured by polyethylene polyamine through covalent reaction to form a stable amid bond. Then, a benzimidazole bond was formed between DABA and −CHO of 5fdUTP, and 5fdUTP was selectively captured on the electrode. Using b-TiO2 as a cross-linker, a guanine-rich ssDNA sequence was further immobilized on the electrode surface by covalent reaction with the 5fdUTP phosphate group. With the assistance of K+ and hemin, the hemin/G-quadruplex structure was formed on the electrode. The hemin molecules in the structure of hemin/G-quadruplex obviously enhanced the PEC response of the biosensor for detecting 5fdUTP, with a linear range of 0.005–500 nM and a detection limit of 1.53 pM (S/N = 3). In addition, this method exhibits optimistic selectivity. The precision and accuracy of this method were evaluated by studying the content of 5fdUTP in genome DNA of crop tissues with standard addition recovery experiments.
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Journal of Materials Chemistry B
·
2021
·Vol. 9
·期 36
·7492-7505
·
IF 6.331
Wendi Ma,Mingjuan Zhou,Wenying Dong,Shanshan Zhao,Yilong Wang,Jihang Yao,Zhewen Liu,Hongshuang Han,Dahui Sun,Mei Zhang
A resveratrol-loaded bi-layered scaffold (RBS) that consists of a resveratrol-loaded poly(lactic-co-glycolic acid) (Res-PLGA) electrospinning nanofiber mat (upper layer) and an alginate di-aldehyde (ADA)–gelatin (GEL) crosslinking hydrogel (ADA–GEL) (lower layer) was fabricated as a wound dressing material. It was made through mimicking the epidermis and dermis of the skin. The RBS exhibited good hemostatic ability and proper swelling ability. Furthermore, HaCaT cells and human embryonic skin fibroblasts (ESFs) were also cultured in the nanofiber layer and hydrogel layer of RBS, and the results indicated that both HaCaT and ESFs could grow well in the materials. The in vivo experiment using a Sprague-Dawley (SD) rat skin wound as a model showed that the RBS could accelerate the wound healing rate compared with the Res-PLGA group and ADA4–GEL6 group. These results indicated that this resveratrol-loaded bi-layered scaffold can be a potential candidate in promoting wound healing.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Qian Li,Jing Hu,Haiqiang Wang,Zhongbiao Wu
Limited light absorption and severe charge recombination have been widely acknowledged as the two main obstacles restricting the application of P25 in NO photocatalytic conversion. In this work, an advanced heterojunction photocatalyst of Bi/BiOI/black TiO 2 was synthesized via an in-situ solid-state chemical reduction method. The black TiO 2 extended the light absorption to the full spectral region. It constructed a direct Z-scheme heterojunction with BiOI nanosheets, not only promoting the charge separation, but also preserving the strong oxidation ability of photogenerated holes in black TiO 2 and strong reducing ability of photogenerated electrons in BiOI. Thus, more •O 2 − and •OH radical could form when Bi/BiOI/black TiO 2 was subjected to visible light irradiation. Besides, the introduced Bi metal nanoparticles could also enhance the light utilization and served as a cocatalyst to accept the electrons. Therefore, enhanced NO photocatalytic oxidation activity was obtained, with the optimal sample Bi/BiOI/black TiO 2 exhibiting a high NO conversion efficiency of ~70% and NO x removal of ~45%. This work may provide a refreshing perspective for the design of heterojunction photocatalysts for efficient NO photocatalytic purification and other photocatalytic applications.
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CRYSTENGCOMM
·
2020
·Vol. 22
·期 8
·1368-1380
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IF 3.117
Hui Zhou,Kaleemullah Kalware,Ming Shen,Songtao Zhong,Yufeng Yao
A series of BiOCOOH and Bi/BiOCOOH heterojunction micro-/nanostructures with various morphologies have been successfully synthesized by a one-step hydrothermal process with the assistance of formamide. The morphology, structure and composition of the as-obtained samples and the effect of formamide were systematically characterized and investigated. The results reveal that formamide plays multiple roles in the synthesis of the BiOCOOH and Bi/BiOCOOH heterojunctions, which acts as the carbon and alkali source. Moreover, the formic acid abundantly provided by the hydrolysis of formamide serves as the reductant and structure-directing agent. The photocatalytic activities of all the catalysts were evaluated by the degradation of rhodamine B (RhB) and reduction of potassium dichromate (K2Cr2O7) under simulated sunlight irradiation. It is found that the photocatalytic activity is closely related to the morphology and composition of the photocatalyst. The well-defined 3D flower-like BiOCOOH prepared at 20 vol% formamide shows a higher photocatalytic activity than the other BiOCOOH samples, which could be attributed to its hierarchical nanostructure, larger specific surface area and stronger adsorption capacity. Meanwhile, the Bi/BiOCOOH heterojunction obtained at 60 vol% formamide shows the best photocatalytic performance due to the increased light absorbance capacity and more efficient separation and transfer of photogenerated carriers with the existence of in situ deposited metallic Bi. Trapping experiments reveal that h+ and ˙O2− are the main active species in the photodegradation process and a possible photocatalytic mechanism is proposed.
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SENSORS AND ACTUATORS B-CHEMICAL
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2020
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IF 7.1
Han Ren,Xuan Liu,Lu Yan,Yuanyuan Cai,Chongyang Liu,Lingxing Zeng,Aihua Liu
The hierarchical porous carbon with high specific surface area was facilely synthesized by calcination of Enteromorpha prolifera (EP), a renewable ocean waste biomass. The resultant carbon exhibited bienzyme mimetic properties including oxidase-like and peroxidase-like activities, which can be regulated by varying carbonized temperature. The reaction mechanism of the oxidase-like activity of EP-based hierarchical porous carbon (EPC) contributes to singlet oxygen and superoxide anions generated during the reaction, while the peroxidase-like activity arises from hydroxyl radicals. Finally, a sensitive colorimetric biosensor for acid phosphatase was explored based on the oxidase-like activity, demonstrating a linear range of 0.5–15 U/L and the limit of detection (LOD) of 0.1 U/L (S/N = 3). A fluorescent biosensor for H 2 O 2 was also developed with the linear range of 0.05–80 μM and a LOD of 0.017 μM (S/N = 3), based on OH produced with the peroxidase-like activity, which react with terephthalic acid to form 2-hydroxyterephthalic acid. Further, incorporated with glucose oxidase, fluorometric sensing of glucose was realized with the linear range of 0.05–10 mM and a LOD of 30 μM. The bi-enzyme mimics also exhibited high reproducibility and stability. Thus, this EPC can be promising candidates for broad applications in sensing, nanomedicine, industrial catalysis and environmental engineering.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
·
IF 16.683
Chun Chen,Ruoyu Fan,Miaomiao Han,Xiaoguang Zhu,Yunxia Zhang,Haimin Zhang,Huijun Zhao,Guozhong Wang
A green process for production of imine and secondary-amine with high selectivity is desirable and challenging. Here, selective production of these nitrogen-containing compounds in one-pot was effectively realized in a hydrogenation-coupling tandem reaction system catalyzed by bi-metallic NiCo catalyst. The investigation of Co/Ni composition vs activity showed a composition-dependence catalysis and the optimal bi-metallic catalyst was NiCo 5 (Ni and Co molar ratio 1:5). Nitrobenzene (NB) could almost completely transform toward imine at 70 °C and secondary-amine at 90 °C, respectively. The adsorption configurations of reactant on catalyst surface were analyzed by DFT calculation to probe the reaction mechanism. And the reaction dynamics were also investigated deeply, suggesting that hydrogenation of NB should be promoted but hydrogenation of benzaldehyde (BA) need inhibiting. Additionally, the catalytic system under moderate reaction conditions could also be applied to a variety of substituted aromatic nitro and aldehyde compounds, showing high yields of corresponding imines.
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