Small Methods
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2020
·Vol. 4
·期 9
·2000208
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IF 12.13
Chaoxiong Zhang,Haoxuan Liu,Yifan Liu,Xijun Liu,Yuying Mi,Ruijie Guo,Jiaqiang Sun,Haihong Bao,Jia He,Yuan Qiu,Junqiang Ren,Xiangjun Yang,Jun Luo,Guangzhi Hu
Using hydrazine oxidation reaction (HzOR) to replace the oxygen evolution reaction is an effective way to decrease the overpotential of the anodic reaction in overall water splitting (OWS), facilitating cost-effective and safe hydrogen production. Herein, Rh 2 S 3 /N-doped carbon hybrids (Rh 2 S 3 /NC) are first reported as novel and efficient bifunctional electrocatalysts for hydrazine-assisted hydrogen generation over a wide pH range. Specifically, Rh 2 S 3 /NC exhibits low overpotentials for the hydrogen evolution reaction (HER) in alkaline (38 mV), neutral (46 mV), and acidic (21 mV) electrolytes, to reach the current density of 10 mA cm −2 , and maintains the activities over 70 h. Meanwhile, Rh 2 S 3 /NC also displays competitive HzOR performance at all-pH electrolytes. Thus, serving as a bifunctional electrocatalyst for both HER and HzOR, Rh 2 S 3 /NC shows overwhelming-Pt/C performance in three electrolytes, and can save over 93.3%, 85.2%, and 78.3% energy consumption compared to the corresponding OWS system. Moreover, theoretical calculations confirm that Rh 2 S 3 /NC owns low free-energy changes of the H adsorption and the dehydrogenation of adsorbed NHNH both of which are beneficial to enhance catalytic activity. This work develops a novel bifunctional electrocatalyst with free pH-dependent condition for the hydrazine-assisted electrolysis system to furtherly reduce the cost of massive industrial H 2 production.
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JOURNAL OF MATERIALS SCIENCE
·
2020
·Vol. 55
·期 17
·7417-7431
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IF 3.553
Meng Xingtong,Jia Shuai,Mo Lanlan,Wei Jie,Wang Feijun,Shao Ziqiang
Nowadays, it has become a trend to prepare porous carbon as electrode materials for supercapacitors by using biomass and its derivatives by virtue of its low cost, abundant source and environmental friendliness. Carboxymethyl cellulose ammonium (CMC-NH 4 ), a kind of cellulose derivative, is used as a carbon precursor and O/N source to prepare carbon material through cross-linking with aluminum ions, lyophilization, carbonization and activation. The as-prepared O/N-co-doped carbon samples (ONAC-500, ONAC-600 and ONAC-700) exhibit hierarchically porous structure with different size pores in carbon framework, ensuring electrolyte ions effective transport and diffusion. Meanwhile, the ONAC-600 reveals a high specific surface area of 2658 m 2 g −1 , abundantly porous structure with pore volume of 1.32 cm 3 g −1 and effective O/N-doping, which ensure a high capacitance of 465.0 F g −1 at 1 A g −1 in 3 M KOH three-electrode system. It also shows better rate capability and good stability after 10000 cycled under 10 A g −1 . Besides, the assembled all-solid-state supercapacitor with ONAC-600 delivers an acceptable energy density of 7.8 Wh kg −1 at a power density of 124.2 W kg −1 .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2020
·
IF 3.573
Meng Chen,Wei Lu,Hejun Zhu,Leifeng Gong,Ziang Zhao,Yunjie Ding
Linear α-olefins (C8–C12 α-olefin, LAOs) are acknowledged as high-value-added chemicals in both lubricant production and the polyolefin industry. An alternative route to the synthesis of high-purity LAOs is the dehydration of linear long-chain n-alcohols, whereas elevating the activity and selectivity of catalysts remains a challenge. Herein, we presented that on using sodium-modified γ-Al2O3 as the catalyst, a high selectivity (up to 96.87%) to 1-decene was achieved, and an optimized experimental condition (329 °C and 0.25 h–1) was found using the response surface method. Characterization results including X-ray diffraction (XRD), Brunauer–Emmett–Teller (BET), pyrolysis (Py)-IR, NH3-temperature-programmed desorption (TPD), and CO2-TPD showed that a suitable ratio (∼0.4 wt %) of sodium impregnation could inhibit the strong acid sites of the catalyst, and sodium impregnation led to the formation of additional base sites, which accounted for the synergistic effect with other acid sites to promote further conversion of ethers to olefins. This work is of significance for the synthesis of LAOs from long-chain n-alcohols.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2020
·
IF 3.807
Xinyu Zheng,Yingcai Hu,Huizi Li,Bolun Han,Ruiyu Lin,Biao Huang
Metal-organic frameworks (MOFs) of type ZIF-67 via simple heat- treatment process was employed to prepare N-doped carbon nanotube frameworks (NCNTFs). Whereafter, an electroanalysis method using NCNTFs as the modify material was constructed for selective sensing of hydroquinone (HQ) and catechol (CC). Both HQ and CC can be independently determined in mixed solutions. The anodic peak currents of HQ increase linearly in two concentration ranges, one from 0.8 to 100 and another from 100 to 200 μM. Also, the anodic peak currents for CC increase linearly in the concentration ranges of 0.8–40 μM and 40–120 μM. The detection limits are 0.17 μM and 0.12 μM for HQ and CC, respectively. The sensor was used to detect these two isomers in spiked lake water, and recoveries for HQ and CC are 91.6–95.0% and 95.3–105.0%, respectively.
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TALANTA
·
2020
·
IF 5.339
Yang Tian,Ruizhi Tang,Luyao Liu,Yang Yu,Shujuan Ma,Bolin Gong,Junjie Ou
Hydrophilic interaction chromatography (HILIC), as one of the important methods for glycopeptides enrichment, has attracted the attention of more and more researchers due to the high efficiency in glycopeptides enrichment. Ordered mesoporous silica materials have been used in many fields, such as catalysis, separation and drug delivery, owing to their adjustable pore size, excellent mechanical properties and ease of preparation. In our case, a series of ordered mesoporous silicas with different pore sizes (3.7–16.7 nm) were prepared via sol-gel reaction employing F127 as the template and TEOS as the silica source. After modified with glutathione by photo-initiated thiol-ene reaction, these materials exhibited hydrophilicity and could be used as adsorbents of HILIC for capturing N-linked glycopeptides from IgG and serum protein tryptic digests. Up to 26 N-glycopeptides were identified from IgG digest, and 565 N-glycopeptides and 330 N-glycosylation sites, mapped to 159 glycoproteins , were identified from 2 μL human serum digest, indicating the great ability for enriching N-glycopeptides from complex biological samples.
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PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yuanyuan Guo,Anrui Dong,Qi Huang,Qipeng Li,Yue Hu,Jinjie Qian,Shaoming Huang
The rational design and preparation of nonprecious metal-based oxygen reduction reaction (ORR) catalysts to facilitate electron and mass transport are of great significance in oxygen-involved energy applications. Herein, a stepwise approach to synthesize a type of hierarchically porous N -doped carbon nanotubes (CNTs) grafted onto zinc-based coordination polymer derived carbon nanomaterials (M−NCNT, M = Fe/Co/Ni) is proposed. At first, an isostructural zinc-based metal–organic framework (MOF) to HKUST-1(Cu) ( ZnHKUST-1 ) is solvothermally prepared, and then under pyrolysis to obtain MOF-derived porous carbon. After the secondary calcination, the in-situ formed N -doped CNTs are efficiently catalyzed by iron group metal-based nanoparticles (Fe/Co/Ni), which are thermally reduced by porous carbon together with additional urea. The synergistic effect between ultrahigh porosity, large surface area, suitable N -doping, high graphitization degree, and ultrafine metal particles prompts M−NCNT series to exhibit satisfactory electrocatalysis in oxygen reduction. Among them, Fe-NCNT owns the optimal ORR activity with high positive onset potential (0.987 V), half-wave potential (0.860 V) and large diffusion-limited current density (4.893 mA cm −2 ). Meanwhile, it shows a high current retention of 90.7% after the 24-hour stability, and the obtained Zn-air battery by Fe-NCNT with open-circuit voltage of 1.44 V owns moderate capacity and satisfying stability. The demonstrated method to prepare hierarchically porous N -doped carbon nanomaterials stemmed from MOF precursors unfolds a new route for the facile construction of efficient nanocatalysts for advanced energy applications.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2021
·
IF 5.455
Ying Shi,Qiuming Zhou,Zhangfeng Qin,Zhiwei Wu,Weiyong Jiao,Mei Dong,Weibin Fan,Jianguo Wang
The aromatization of alkanes is an important process for improving the quality of Fischer-Tropsch synthesis (FTS) gasoline and producing high-valued aromatics from naphtha ; however, currently available catalysts in this regard are often deficient due to the low aromatics yield and short lifetime. In this work, a series of hierarchically structured Beta (Beta-HS) zeolites with high crystallinity and meso-porosity were synthesized by steam treatment with various organosilanes as pore-forming reagent and ethanol as solvent. The nano-sized Beta-HS zeolites were further modified with K through ion-exchange and with Pt through incipient wetness impregnation; the resultant Pt/K-Beta-HS catalysts were then used in the aromatization of n -heptane. The results indicate that the abundant mesopores present in Beta-HS are conducive to the diffusion of reactants and products, whilst the modification with K is able to passivate the strong Brønsted acid sites and the loading of Pt metal can promote the dehydrogenation of alkanes and cycloalkanes, which can effectively suppress the cracking and carbonaceous deposition reactions and enhance the dehydrogenation aromatization activity. As a result, the Pt/K-Beta-HS catalysts exhibit excellent performance in the aromatization of n -heptane, with a much longer lifetime (205 h), higher selectivity to aromatics (80%) and larger turnover number of aromatic products (Pt-based TON, 240 × 10 3 ) than conventional Beta zeolites. These results prove that the steam treatment with organosilanes as pore-forming reagent is a facile and cost-effective strategy to synthesize the hierarchically structured Beta zeolites and after loading K and Pt, the Pt/K-Beta-HS zeolites can be an efficient catalyst for the conversion of n -heptane to aromatics.
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Progress in Natural Science-Materials International
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2021
·
IF 3.607
Xinxin Jin,Yan Xie,Chaoyue Zhao,Yinghao Xu,Yang Lv,He Wang,Li Chen,Jiahui Huang
FeCo-based non-noble metal electrocatalysts (NNMEs) of FeCo/MCS-NPCS was fabricated by immobilization of hemin on mesoporous carbon shells modified N-doped porous carbon spheres (MCS-NPCS). The obtained FeCo/MCS-NPCS exhibits a half-wave potential (E 1/2 ) of 0.851 V versus the reversible hydrogen electrode (vs. RHE) and a limited-diffusion current density (J L ) of 5.45 mA cm −2 . In addition, FeCo/MCS-NPCS shows comparable oxygen reduction reaction (ORR) performances to 20 wt% Pt/C in terms of E 1/2 and J L and better electrochemical properties, including the methanol tolerance and durability in alkaline solution. Such outstanding electrochemical activities of FeCo/MCS-NPCS can be ascribed to Fe and/or Co-based nitrides and carbides as well as N-doped carbon matrixes modified with mesoporous carbon shells. This research introduces a promising path to design and synthesize highly efficient FeCo–N–C electrocatalysts towards ORR.
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JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2021
·
IF 5.541
Fanggang Liu,Lijun Jin,Yanpeng Ban,Haoquan Hu
To understand the pyrolysis behavior of long linear alkanes, six n-alkanes (n-C n H 2n+2 , n = 10, 12, 13, 14, 15, 16) were conducted by pyrolysis coupled with photoionization molecular-beam mass spectrometer at pressure below 10 Pa and temperature between 200 °C and 1000 °C. Lots of important alkyl and alkenyl radicals (CH 3 , C 4 H 9 , C 8 H 15 , C 9 H 19 , C 3 H 5 , C 5 H 9 , etc.), which are the direct evidence to understand the pyrolysis reaction pathway, were real-time detected by mass spectral detector. The results suggested that the predominant pyrolysis mechanism of n-alkanes is a free-radical chain mechanism, beginning with the C C bond homolysis of n-C n H 2n+2 to produce primary alkyl radicals (C m H 2m+1 , m < n) and termination by β C-H homolysis and mutual combination of radicals. The chain is propagated by the β C-C homolysis and H-abstraction of primary alkyl radicals to produce secondary alkyl radicals (C h H 2h+1 ), and then the β C-C homolysis and H-abstraction of the secondary alkyl radicals to form alkyl/alkenyl radicals (C h H 2h+1 /C k H 2k-1 , h ≤ n, k < n-3) and alkenes (C k H 2k /C k H 2k-2 ) and the hydrogen-shift to form free-radical isomers. During the process, H-abstrction, and hydrogen-shift reactions exist as a synergistic reaction. In addition, the position of free radical in alkyl isomers is closer to the central carbon at low temperature. With the increase of temperature, 2-C m H 2m+1 radical are gradually dominated.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yi Wang,Qingjie Ji,Jixiang Xu,Jun Wan,Lei Wang
In this study, N-doped porous carbon materials embedded with NiN x species (Ni@NC) were fabricated via the pyrolysis of Ni-doped zeolitic imidazolate frameworks-8 (ZIF-8) at the temperature of 900 °C. The obtained Ni@NC-1 catalyst exhibited excellent activity in activating the peroxydisulfate (PDS) that was used for removing tetracycline (TC). The catalytic system exhibited good stability, wide pH adaptation, and high resistance to the operational environment. It was supposed that NiN x species could attach to PDS and act as electron acceptors to receive the electrons for activating the PDS, thus generating highly reactive superoxide radicals (⋅O 2 − ) and singlet oxygen ( 1 O 2 ) species for rapid degradation of TC. The electron transfer and dissolved oxygen-derived ⋅O 2 − were also responsible for the degradation of TC. In addition, the Ni@NC-1/PDS system exhibited high efficiency for removing oxytetracycline, ciprofloxacin, or levofloxacin. The results of this study would promote the design of other MOFs-derived carbon-encapsulated metal species for efficiently activating persulfate to remove antibiotics from the wastewater.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Yuting Zeng,Yan Li,Xiaofeng Tan,Jindi Gong,Ziyu Wang,Yuhao An,Zhenqiang Wang,He Li
Among plentiful porous nanomaterials, noble metal aerogels taken as nanozymes attract broad attention in sensing applications with their distinct enzyme mimic functions. In the catalytic field, the heteroatom doping strategy is a kind of way with great promise in improving the enzyme mimic activity of noble metal aerogels. In this experiment, we find a type of creative materials that were prepared by the fast and simple method. Due to the unique porous structure and synergetic effect from doped atoms, PdRu aerogels co-doped with boron and nitrogen (B, N-PdRu aerogels) were prepared using NH3BH3 as a reductant, which present improved peroxidase mimicking activity. With the existence of H2O2, the oxidation of 3,3′,5,5′-tetramethylbenzidine was catalyzed by B, N-PdRu aerogels fairly efficiently, whose solution would be a blue appearance at optimum absorption wavelength 652 nm. Thus, by the tandem reaction bound to the enzyme glucose oxidase, the B, N-PdRu aerogels can be used for the sensitive determination of glucose. The new method has a good linear detection effect for glucose in the range of 10 μM to 2 mM. The minimum limit of detection can reach as low as 6 μM. This work will contribute to research on the rational design of metal aerogels based on the heteroatomic doping strategy and enhance the corresponding performance for a variety of applications.
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高影响因子
IONICS
·
2021
·Vol. 27
·期 10
·4461-4471
·
IF 2.817
Zeng Depeng,Shu Dong,Yi Fenyun,Gao Aimei
A nest-like N-doped hierarchical porous active carbon (N-HAC) with higher specific surface area is achieved successfully by melamine cyanurate (MCA) sacrifice template molding and assistant chemical activation of NH 4 Cl and CaCl 2 . The results testify that the nest-like hierarchical porous character of N-HAC can form an interconnecting structure and introduce plenty of supercapacitor reactive sites, which can facilitate the ion diffusion/migration among the material, while nitrogen doping in N-HAC can change the charge distribution of N-HAC and then promote the electron transfer. Attributing to the synergistic effect of the hierarchical porous structure and nitrogen doping, N-HAC800 displays the highest specific capacitance (284.6 F g −1 at 1 A g −1 and 183.1 F g −1 even at 20 A g −1 ) and superior cycle stability (80.4% after 5000 cycles at 100 mV s −1 ). This study results prove that the N-doped hierarchical porous active carbon is a promising material for energy storage application in the future.
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