Catalysis Science & Technology
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2020
·Vol. 10
·期 5
·1336-1342
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IF 5.721
Ziqi Zhang,Kaida Yao,Linchuan Cong,Zhuochen Yu,Lina Qu,Weimin Huang
Ammonia is one of the most important agricultural fertilizers and renewable energy carriers, and is also one of the most highly produced inorganic compounds in the world. The traditional industrial ammonia synthesis mainly uses the Haber–Bosch method, which consumes a large amount of fossil fuels and emits a lot of greenhouse gas. Thus, a more environmentally friendly method is needed for the production of ammonia. In this paper, we present a new electrocatalyst to produce NH3 under ambient conditions, which was obtained via the carbonization of Ru-dispersed ZIF-8. As a result, the catalyst could achieve a maximum NH3 production rate of about 16.68 μgNH3 h−1 mgcat.−1 at −0.4 V (vs. RHE) and a faradaic efficiency of 14.23% at −0.3 V (vs. RHE) at room temperature and ambient pressure in 0.1 M KOH. Also, the loading of Ru is only 16 wt%. Thus, this work provides a feasible method to design highly dispersed noble metal electrocatalysts for the nitrogen reduction reaction (NRR).
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SENSORS AND ACTUATORS B-CHEMICAL
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2019
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IF 6.393
Feifei Zhao,Tianyi Zhang,Qian Liu,Changli Lü
For most of the carbon dots (CDs), solid-state fluorescence and room temperature phosphorescence (RTP) are difficult to achieve due to self-quenching and intersystem crossing (ISC) limitations. Here, nitrogen-doped CDs-1 showing both fluorescence and RTP was obtained by hydrothermal reaction from polyvinyl alcohol (PVA) and 5-amino-1,10-phenanthroline (Aphen). The CDs-1 emits blue-green fluorescence in aqueous solution, while emits white fluorescence and yellow-green RTP in the solid state with a RTP lifetime up to 103 ms, exhibiting a long afterglow with a duration of 3 s, which is visible to the naked eyes. The RTP of the CDs-1 is derived from the C N/C N in Aphen and C N/CN in Aphen and C O produced during the carbonization process with a small energy gap between the singlet and triplet states, which helps to realize the ISC. At the same time, the hydrogen bonds between the C N/CN or CO bonds and O H of the not completely carbonized PVA chains on the CDs-1 surface have the advantages of moisture resistance, oxygen barrier and improving the rigidity of CDs-1. Eventually, non-radiative transitions can be suppressed. Based on the decent fluorescence properties, the aqueous solution of CDs-1 can be used to detect TNP and is responsive to pH with a good linear relationship between acid and alkali. In addition, the RTP of CDs-1 can be utilized as banknote anti-counterfeiting material under a long excitation wavelength. This work provides a possibility to realize the multi-mode illumination regulation of CDs by facile one-step strategy.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
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IF 6.361
Xinxin Zhu,Yabo Li,Rong Li,Keke Tu,Junsheng Li,Zhizhong Xie,Jiaheng Lei,Dan Liu,Deyu Qu
Lithium-sulfur batteries hold broad prospects as the low-cost and high-energy storage system. However, the practical application is limited by the intrinsic insulating nature of sulfur and severe shuttle effect of soluble polysulfide intermediates. Herein, we demonstrate a convenient self-assembly strategy for encapsulating carbon nanotubes in nitrogen-doped hollow carbon shells, to construct a nitrogen-doped tube-in-tube carbon nanostructure (NTTC) as a host material of sulfur. In this peculiar structure, the highly conductive carbon nanotube cores facilitate the electron transfer while the hollow porous structure is capable of accommodating high sulfur content of 70 wt% in the composites. Moreover, the nitrogen doping helps to alleviate the shuttle effect owing to enhanced chemisorption towards polysulfides. Benefiting from these merits, the NTTC/S composite with the high areal mass loading of ~2.5 mg cm −2 presents a high reversible capacity (1346.9 mAh g −1 at 0.05 C) and excellent rate capability (533.5 mAh g −1 at 3C). More impressively, NTTC/S electrode exhibits good cycling stability at a high rate of 2 C corresponding to slight capacity decay of 0.055% per cycle over 500 discharge/charge cycles.
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RSC Advances
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2019
·Vol. 9
·期 69
·40222-40227
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IF 3.049
Yongping Wang,Qiaoli Yue,Yingying Hu,Chen Liu,Lixia Tao,Cong Zhang
N-doped carbon dots (NCDs) exhibit bright blue emissions and have been used as viable fluorescent probes in the turn-off fluorometric assay for vanillin detection. NCDs were prepared from glucose and tyrosine using a facile and green synthesis process. The one-pot hydrothermal treatment was used without any strong acid or oxidant. The fluorescence of NCDs (with excitation/emission peaks at 323/416 nm, respectively) can be quenched by vanillin. The quenching mechanism belongs to the dynamic quenching mode due to the molecular collisions of the ground state of vanillin and the excited state of NCDs. This turn-off system could be utilized to quantify vanillin within a linear range of 0.43–264 μM. The limit of detection was 0.10 μM. Moreover, this approach was successfully applied toward the determination of vanillin in food samples.
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JOURNAL OF SOLID STATE CHEMISTRY
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2019
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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
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2019
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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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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 COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Zhefu Li,Binling Chen,Xianfeng Wang,Jun Nie,Guiping Ma
In this work, a novel catalyst of oxygen reduction reaction (ORR) was designed and fabricated by electrospinning, photo-curing and carbonization, based on polymer poly(dimethylsilylene ethynylenephenyleneethynylene) (PMSEPE) and metal organic frameworks (MOFs)—Materiaux de l'Institute Lavosier-101(Fe) (MIL-101(Fe)). The optimal catalyst PMSEPE/MIL-101(Fe)-800, which was carbonized at 800 °C, presented a bamboo-like nanofiber structure with a high degree of graphitization, a high specific surface area (302.3 m 2 /g) and a high yield (64.17%). Fe 3 C particles were found to be encapsulated into the Fe-Si-N co-doped carbon nanofibers. In the electrochemical tests, PMSEPE/MIL-101(Fe)-800 showed an onset potential of 0.935 V ( vs . RHE) and a diffusion limit current of 6.01 mA/cm 2 ( vs . RHE) in 0.1 M KOH aqueous solution, of which performances are competitive to commercial 20 wt% Pt/C. PMSEPE/MIL-101(Fe)-800 also exhibited a higher methanol tolerance and duration stability. Further Zn-air battery test used by PMSEPE/MIL-101(Fe)-800 suggested its potential for the application of fuel cell.
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ACS Applied Nano Materials
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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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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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2019
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IF 4.084
Yang Hui Deng,Bai Xiang Tao,Cui Ye,Qing Zhang,Guo Chen,Xiao Hu Wang,Yan Shi,Jing Rong Chen,Hong Qun Luo,Nian Bing Li
Developing the cost-effective catalyst based on earth-abundant materials is a crucial demand for water oxidation . Doping heteroatom into catalysts is regarded as an effective strategy to regulate electronic configuration and improve the catalytic performance of water oxidation. In this work, N-doped CoS 2 on carbon cloth is fabricated by one-step synthesis, in which thiourea acts as both sulfur and nitrogen sources. The N-doped cobalt disulfide shows superior catalytic activity for oxygen evolution, with a low overpotential of 240 mV for 10 mA cm −2 , small Tafel slope (56 mV dec −1 ) and high turnover frequency due to the modification with electronic structure after incorporation of N atom. Moreover, the incorporation of N atom provides a distinctive perspective of doping other heteroatom into the material for modifying the electrochemical properties .
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APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Xueping Dai,Yan Wang,Xiao Wang,Shengrui Tong,Xiaofeng Xie
The surface adsorption is considered to be a very important factor in photodegradation process, especially in the removal of gaseous pollutants. In this work, nitrogen doped reduced graphene (N-GR)/TiO 2 were synthesized to probe the polarity adsorption and photodegradation characteristics of acetaldehyde (polar) and ethylene (nonpolar). Morphology and properties of the samples were revealed by TEM , Raman spectra , photoluminescence spectra, photocurrent , electron spin resonance and so forth. Adsorption of flowing gas and TPD were used to indicate the adsorption ability of the composites towards acetaldehyde and ethylene. In experiments, the difference of nitrogen doping amount can adjust the polarity of N-GR/TiO 2 composites efficiently and then influence their photodegradation performance. Specifically, the N-GR/TiO 2 showed higher acetaldehyde adsorption capacity than GR/TiO 2 , while the GR/TiO 2 possessed the highest adsorptive abilities in ethylene case. In the subsequent photodegradation tests of flowing acetaldehyde, all of the N-GR/TiO 2 samples had removal efficiencies higher than that of GR/TiO 2 . The highest removal efficiency reached by the 2 N-GR/TiO 2 is around 82%. In the ethylene to contrast, the removal efficiency was obtained as 93.8% by GR/TiO 2 , which is higher than that of the N-doped samples. It can be seen that the high polarity samples could improve the adsorption and photodegradation performance of polar molecules , which could propel the understanding and application of photodegradation technologies.
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