Inorganic Chemistry Frontiers
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2023
·Vol. 10
·期 8
·2370-2379
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IF 7
Yanli Ruan,Hang Xu,Haikuo Lei,Wenjuan Xue,Tianyu Wang,Shidong Song,Yangyang Yu,Gui-Rong Zhang,Donghai Mei
Zn–air batteries (ZABs) have been widely studied due to their high theoretical energy density, low cost, and high safety. However, the lack of efficient bifunctional electrocatalysts toward both the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) hinders their large-scale application. Herein, a dendritic NiS2@Co–N–C/CNF nanoarchitecture is proposed, which was fabricated by high-temperature carbonization of Co-MOFs and a subsequent simple hydrothermal composite method using NiS2 nanosheets. The catalyst is reasonably designed to integrate the oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) active sites on the surface of carbon nanofibers. Through the synergy between NiS2 and Co–N–C/CNF and the unique branch–leaf porous structure, the catalyst showed excellent catalytic activity and stability. In an alkaline electrolyte, the OER overpotential of NiS2@Co–N–C/CNF is 300 mV at 10 mA cm−2. The ORR half-wave potential (E1/2) of NiS2@Co–N–C/CNF is 0.8 V. In addition, the superior catalytic activity of NiS2@Co–N–C/CNF could be transferred to a ZAB, which exhibits a maximum peak power density of 181 mW cm−2 along with an ultra-long cycling stability for 1050 and 600 h at discharging current densities of 5 and 10 mA cm−2, respectively. The performance is significantly higher than that of commercial precious metal Pt/C + IrO2 mixed catalysts. The peak power density of solid state ZAB (SSZAB) integrated with NiS2@Co–N–C/CNF is 76 mW cm−2, and it can still maintain excellent cycling stability under different bending states. More impressively, four in-series SSZABs (NiS2@Co–N–C/CNFs) can charge smartphones, indicating their potential feasibility in the field of wearable electronics.
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ACS Applied Materials & Interfaces
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2023
·
IF 9.5
Limin Wang,Wenhui Song,Stephen Choi,Kai Yu,Feng Zhang,Wei Guo,Yajie Ma,Kai Wang,Fengyu Qu,Huiming Lin
Sonodynamic therapy (SDT) can be described as ultrasonic (US) catalysis. Adequate charge separation is considered as effective means to promote reactive oxygen species (ROS). Here, hollow CoP@N–carbon@PEG (CPCs@PEG) nanospheres (∼60 nm) are prepared as sonosensitizers, showing greater ROS generation than pure CoP@PEG under US irradiation. Both 1O2 and ·O2– are activation species that are determined by O2 and electrons. The great SDT performance of CPCs@PEG is ascribed to the heterostructure which promotes the separation and transfer for US-generated electrons and holes. In addition, holes can be further captured by endogenous glucose that is in favor of electron aggregation and ROS generation. Moreover, the consumption of glucose would decrease intracellular ATP for starvation therapy. Given the higher oxidation ability of Co3+, CPCs@PEG nanospheres possess catalase (CAT) activity to convert H2O2 into O2 for assisting ROS generation. Moreover, they also can oxidize glutathione (GSH) as a mimic GSH oxidase to break intratumor redox balance, facilitating oxidative stress. More importantly, the nanocomposites reveal good degradation ability dominated by the oxidation from insoluble phosphide into soluble phosphate, accelerating elimination via urine and feces within 14 days. CPCs@PEG nanospheres integrate the above effects not only to reveal great tumor inhibition ability but also to excite immune activation for anticancer.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2019
·
IF 3.218
Li Liu,Sadat Anwar,Haizhen Ding,Mingsheng Xu,Qiang Yin,Yazhong Xiao,Xingyuan Yang,Manqing Yan,Hong Bi
Carbon dots (CDs) as a new type of carbon nanomaterial have gained tremendous attention due to their wide applications in photocatalyst, sensor, bioimaging and so on. In the present work, a novel kind of fluorine and nitrogen co-doped CDs (F,N-CDs) have been synthesized from 5-fluorouracil (5-Fu) and p -phenylenediamine ( p -PD) via a hydrothermal method . An electrochemical sensor for detecting catechol was designed and constructed on the basis of F,N-CDs and laccase (Lac). Compared with the traditional detection methods of catechol, the as-fabricated sensor Lac-F,N-CDs/glassy carbon electrode (GCE) shows a comparatively low detection limit (0.014 μM) as well as a high sensitivity (219.17 μA cm −2 mΜ −1 ) through the amperometric i-t responses method. The most significant feature of the sensor is its long cycle stability and can be used for many times (≥50) under ambient conditions. The prepared Lac-F,N-CDs/GCE sensor has been employed for detection of catechol in tap water and lake water successfully. This work provides a new pathway to stabilize laccase by using CDs and other carbon nanomaterials to construct efficient electrochemical sensor for detecting catechol and its analogue.
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JOURNAL OF SOLID STATE CHEMISTRY
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2019
·
IF 2.291
Yu Sang,Hansheng Li
The objective of this work is to investigate the catalytic effect of a series of modified HZSM-5 zeolites on n-decane cracking at 500 °C and atmospheric pressure. The zeolite catalysts were prepared with phosphorus and/or mesopore modification by excessive impregnation and/or hydrothermal treatment , and were characterized with various methods including SEM, TEM , XRD , FTIR, N 2 adsorption-desorption measurement and NH 3 -TPD. Results show that the addition of phosphorus adjusted the distribution and strength of acid sites in the zeolite crystals. The introduced mesoporous structure improved the diffusion of reactants and products in zeolite pores during n-decane cracking. With appropriate acid amounts and distribution, as well as short channels and high specific surface area, the modified HZSM-5 nanoparticles exhibited higher catalytic activity, better light olefins selectivity and longer lifetime, compared with the original HZSM-5 zeolite. The phosphorus modified HZSM-5 zeolites coupling with MCM-41 matrix was proved to be a promising catalyst for the thermal cracking of n-decane.
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ANALYTICA CHIMICA ACTA
·
2019
·
IF 5.256
Fengjuan Ding,Zhanying Chu,Quanqing Zhang,Haiyan Liu,Weibing Zhang
Hydrophilic interaction liquid chromatography is a significant strategy for the separation and enrichment of glycoproteins and glycopeptides . A layered imine-based covalent organic polymer with mesopores (denoted as p-TpBDH) was successfully fabricated by a facile solvothermal method . Then p-TpBDH-OH with abundant hydrophilic groups was evolved from p-TpBDH by the direct reduction. 36 and 40 glycopeptides were identified from IgG digests respectively by p-TpBDH and p-TpBDH-OH. Furthermore, the p-TpBDH-OH exhibits superior selectivity (IgG: BSA = 1: 250) for glycopeptides compared with the p-TpBDH. Encouragingly, a total of 463 glycopeptides assigned to 173 glycoproteins were finally identified from only 2 μL human serum by the p-TpBDH-OH. Compared with p-TpBDH, abundant hydrophilic and nitrogen-containing affinity sites of p-TpBDH-OH facilitate effective hydrophilic interaction between the polymeric material and glycopeptides. All the results demonstrate the functionalized hydrophilic covalent organic polymer has great potential in large-scale N-glycoproteomic research.
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SPECTROCHIMICA ACTA PART A-MOLECULAR AND BIOMOLECULAR SPECTROSCOPY
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2019
·
IF 2.931
Hongwei Hu,Xinmeng Tian,Yixuan Gong,Guolan Ren,Jiangong Liang
Despite extensive research on carbon dots (CDs), rare studies have been performed on the photostability of CDs. Here, the photostability of CDs synthesized with 3-aminobenzoic acid were systematically investigated under different pH conditions (5.0, 7.4 and 9.0). The results showed that under Xenon lamp irradiation, the fluorescence (FL) intensity of the CDs exhibited an increase first and then a decrease, with a gradual shift of the maximum emission wavelength to longer wavelength. Further investigation indicated that the irradiation induced the change of the CD surface functional groups and gave rise to aggregation, resulting in the formation of larger particles. This study provided important reference value towards research on CDs properties.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2018
·
IF 4.229
Zhao Jiang,Xiang Gong,Bin Wang,Zhiqiang Wu,Tao Fang
Liquid organic hydrogen carrier (LOHC) is considered as a promising candidate for large-scale hydrogen storage. In this work, we found that Pt/TiO 2 catalysts exhibited better catalytic activity and selectivity compared to Pd/TiO 2 and commercial Pd/Al 2 O 3 catalysts in the dehydrogenation of dodecahydro-N-ethylcarbazole (12H-NECZ) at 453 K. The catalytic activity of the noble metal catalysts followed the trend of Pt/TiO 2 > Pd/TiO 2 > Rh/TiO 2 > Au/TiO 2 > Ru/TiO 2 . Compared with the commercial Pd/Al 2 O 3 , Pt/TiO 2 greatly improved the selectivity and conversion rate, the reaction time was also shortened. In addition, kinetics calculation was carried out to obtain fundamental reaction parameters. It was found that the third step of 4H-NECZ dehydrogenation to NECZ was the rate-limiting step of the entire dehydrogenation reaction for all catalysts.
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CARBON
·
2019
·
IF 7.466
Xiaoqing Cui,Xiaohui Liang,Jiabin Chen,Weihua Gu,Guangbin Ji,Youwei Du
Here, we report a unique core-shell nanocomposite of Fe 2 N@N-doped carbon that coats dopamine-derived carbon shells on porous Fe 2 N nanoparticles via a facile and effective soft chemical method . The feasibility of preparing core-shell structure in the process of polymerization is realized by utilizing the fact that affluent amino and hydroxyl groups in dopamine endow the formidable chelation ability with metal ions. Temperature-dependent volume shrinkage effect of Fe 2 N originates from the lattice transformation in nitridation process, which is the key factor to control the void space inside carbon nanocubes and optimize the electromagnetic performance. Consequently, the as-prepared samples achieve excellent reflection loss (RL) values and effective absorption bandwidth at an even thin thickness of 1.4 mm. The balance between the temperature-dependent conduction loss and the optimization of hole structure impedance matching may be responsible for the excellent microwave behaviors. This work offers an attractive core-shell Fe 2 N@carbon with controllable void space as a promising candidate to handle the electromagnetic interface (EMI) issues.
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ACS Applied Nano Materials
·
2019
·
IF 0
Chenxue Yao,Qiang Zhang,Yan Su,Lijian Xu,Hua Wang,Jinglei Liu,Shifeng Hou
A new type of microsphere of graphene oxide (GO) encapsulated zeolitic imidazolate framework-8 (ZIF-8) was prepared through spray-drying methodology, and hollow N-doped graphene microspheres (ZGC) were then obtained by the calcination of the ZIF-GO (ZG) composite microspheres. The ZGC can be used as a supporting material anchoring Pd nanoparticles for ethanol oxidation reaction (EOR). This novel ZGC precursor offers several advantages over other materials. (i) The three-dimensional (3D) hollow structure contains highly order nanoporous, and nitrogen doped structures offer more activity sites for support catalysts and provide more space for catalysis reaction. (ii) The unique 3D structure can avoid the aggregation and deactivation of catalysts. (iii) The conversion of nanostructure of graphene and nanocarbon to microsphere structure offers easy handle process. The optimized ZGC has a high orderly hierarchical pore structure, and Pd/ZGC electrocatalyst shows higher electrocatalytic activity (2490 mA mg–1) than Pd/ZIF (1494 mA mg–1), Pd/rGO (1232 mA mg–1), and Pd/C (467 mA mg–1). The advanced electrocatalytic performance of Pd/ZGC can be ascribed to the particular architecture of ZGC, which will have a wide application prospect in direct ethanol fuel cells (DEFCs).
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ACS Applied Bio Materials
·
2018
·
IF 0
Jianjun Luo,Xing Zhang,Jeremiah Ong’achwa Machuki,Chengbai Dai,Yang Li,Kaijin Guo,Fenglei Gao
Composite biomaterials with hierarchical structures have emerged as new approaches for bone-tissue engineering. In this study, a biomimetic, osteoconductive tricomposite scaffold made of N-doped graphene–hydroxyapatite (NG–HA) hybrids blended with an agarose (AG) matrix was prepared via a facile hydrothermal/cross-linking/freeze-drying method. The structure and composition of AG/NG–HA were examined by scanning electron microscopy, X-ray photoelectron spectroscopy, X-ray diffraction, Fourier transform infrared, Raman spectroscopy, and thermogravimetric analysis. The as-prepared scaffolds showed hierarchical pore architecture and an organic–inorganic composition, which simulated the composition and structure of natural bone tissue. The effect of AG/NG–HA on bone mesenchymal stem cells (MSCs) osteoblast proliferation, differentiation, and mineralization was tested in vitro. The expression of osteogenic-related genes was determined by real-time polymerase chain reaction. Our results showed that the introduction of N-graphene into the hybrid scaffold significantly improved its mechanical properties, an effect that promoted the proliferation and viability of MSCs. Moreover, the scaffolds triggered selective differentiation of MSCs to osteogenic lineage while conferring good cell adhesion, enhanced alkaline phosphatase activity, and mineralization. A distal femoral condyle critical size defect in rabbits was used as a platform to confirm the effect of AG/NG–HA on bone regeneration in vivo. Our experiments show that the AG/NG–HA hybrid scaffolds provided a favorable environment for new bone formation. The results presented in this study suggest that the AG/NG–HA hybrid scaffolds have potential in bone-tissue regeneration engineering.
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ELECTROCHIMICA ACTA
·
2018
·
IF 5.116
Chao Li,Jing Xue,Ao Huang,Jing Ma,Fangzhu Qing,Aijun Zhou,Zhihong Wang,Yuehui Wang,Jingze Li
Owing to the unique redox reaction and the relative low molar mass of the repeating unit, poly(N-vinylcarbazole) (PVK) was selected as an advanced organic cathode for potassium-ion-based dual-ion battery (PDIB) with the K foil anode and KPF 6 -based electrolyte. The operation mechanism of this PDIB is that PF 6 − anions are migrated from the electrolyte and incorporated into PVK cathode via the attraction to the positively charged N atom of carbazole ligand, and then are released into the electrolyte in the subsequent discharge process; simultaneously, K + cations are reversibly stored/removed in/from the anode during charging/discharging. It shows a high median operation potential of 4.05 V vs. K + /K and can achieve a high specific capacity of 117 mAh g −1 at 20 mA g −1 , which is close to its theoretical value of 138 mAh g −1 . More impressively, even at the highest current density of 2000 mA g −1 for 500 cycles, a high average specific capacity of 61 mAh g −1 can still be obtained with capacity rentation of 55%.
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JOURNAL OF MATERIALS SCIENCE
·
2018
·Vol. 54
·期 6
·4589-4600
·
IF 2.993
Tan Jiabin,He Xiaobo,Yin Fengxiang,Liang Xin,Chen Biaohua,Li Guoru,Yin Huaqiang
In this study, a β-Mo 2 C/N, P-co-doped carbon (NPC) catalyst with a porous structure of β-Mo 2 C nanoparticles loading on NPC matrix was prepared by vacuum-rotary evaporation and followed by a facile pyrolysis process for hydrogen evolution reaction (HER). The porous structure is beneficial for exposing more active sites and the mass transfer during the HER. In addition, the carbon matrixes with the highly doped N and P heteroatoms also provide their positive contributions to its high catalytic activity for HER. Owing to the advantages mentioned above, the optimized catalyst shows a small overpotential of 181 mV for driving a cathodic current density of 10 mA cm −2 , a low Tafel slope of 65.3 mV dec −1 and a high exchange current density of 1.5 × 10 −2 mA cm −2 during HER processes in acid electrolyte. The excellent performance of the β-Mo 2 C/NPC makes it a great potential candidate as the HER electrocatalyst.
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