Advanced Sustainable Systems
·
2022
·Vol. 6
·期 3
·2100380
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IF 6.737
Zhengyi Li,Hu Li,Song Yang
Catalytic upgrading of CO 2 into value-added chemicals to build the excess carbon cycle is of great significance. In this work, carboxylate-functionalized zeolitic imidazolate framework (F-ZIF-90) with good crystallinity and porosity is constructed from ZIF-90 and employed as a robust heterogeneous catalyst to boost the reductive N -functionalization of various amines with CO 2 to furnish N -formyl compounds (up to 99% yield) in the presence of PhSiH 3 under an ambient environment. The imidazole carboxylate species ( COO - ) can not only activate hydrosilane and CO 2 to form the key intermediate formoxysliane but also activate amines to participate in the N -formylation reaction to obtain the target product. Moreover, it can enhance the catalyst capture and exchange ability toward ambient CO 2 . The powerful adsorption capacity of the F-ZIF-90 catalyst toward CO 2 is conducive to elevating CO 2 concentration around the active species. Theoretical calculations show that the carboxylate-mediated conversion path undergoes the transition state of hydrosilane activation with a relatively lower energy barrier (Δ G = 26.9 kcal mol –1 ). F-ZIF-90 exhibits good thermochemical stability with no obvious activity attenuation after repeated use 5 times. This strategy opens a new avenue based on ZIFs to develop heterogeneous catalysts for reductive upgrading of CO 2 .
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2015
·
IF 2.999
Lin Chen,Huibo Wang,Chengzhan Liu,Xianchun Liu,Shuangxi Xing
Highly dispersible copper nanoparticles (CuNPs) anchoring on the N-doped carbon films are achieved by pyrolyzing urea, citric acid and copper nitrate in one pot. The presence of the CuNPs and the N-doped carbon film is investigated by transmission electron microscopic, X-ray diffraction, X-ray photoelectron and Raman spectra. The citric acid is used as a carbon source to support the as-synthesized CuNPs and the urea takes a role as a nitrogen source to dope into the carbon structure and localize the CuNPs with a separated state. Such an N-doped carbon film with well-dispersed CuNPs on its surface presents an excellent catalytic performance and stability via using the reduction of 4-nitrophenol by NaBH 4 as a model reaction.
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ACS Sustainable Chemistry & Engineering
·
2020
·
IF 7.632
Cong Huang,Lirong Zheng,Wenshuai Feng,Aimin Guo,Xiaohui Gao,Zhen Long,Xiaoqing Qiu
In recent years, metal isolated site catalysts with the high exposure and maximized availability of metal species provide a new route to boost the oxygen reduction performance. However, in the absence of clusters and nanoparticles, the synthesis of this catalyst with metal high-loading, especially for copper, is still a big challenge. In this work, a metal isolated site catalyst with high copper content (1.12 wt %), copper isolated sites anchored on N-doped carbon materials (donated as Cu ISs/NC-1000), was prepared by the pyrolysis of copper acetylacetone within the metal–organic framework (ZIF-8) at 1000 °C. The successful preparation of products can be demonstrated by high-angle annular dark-field scanning transmission electron microscopy and X-ray absorption spectra. With the merits of the atomically dispersed surface metal atoms and abundant ORR-favored copper active sites, the present Cu ISs/NC-1000 exhibits an excellent ORR electrochemical activity with a half-wave potential of 0.855 V (vs RHE) and a limiting current density of 5.2 mA cm–2 in the electrochemical tests, superior to the results from commercial Pt/C and previously reported Cu-based materials. For the durability, the negligible activity decay after 10,000 continuous potential cycles and good resistance to methanol crossover can be noted. The outstanding catalytic activity from the present Cu ISs/NC-1000 demonstrates the superiority of metal isolated sites as electrocatalytic centers.
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MATERIALS LETTERS
·
2020
·
IF 3.204
Haiyan Zhang,Sen Liu
SnO 2 /Co 3 O 4 n-p heterojunctions have been prepared by organometallic chemistry-assisted approach, where holy Co 3 O 4 nanosheets and (CH 3 ) 2 SnCl 2 were used as precursors. It is found that the surface oxygen-containing species could be regulated by changing the ratio of Co 3 O 4 precursors and Sn-containing organic compound. Our present work is of importance because it provides a new and effective approach for construction of heterojunctions .
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PLASMA SCIENCE & TECHNOLOGY
·
2022
·Vol. 24
·期 4
·044008
·
IF 1.842
Yufa ZHOU,Jingsen ZHANG,Guangqing XIA,Yue HUA,Yanqin LI,Jixiang HU,Xiuling ZHANG,Lanbo DI
In this work, N-doped graphite oxide (GO-P) was prepared by cold plasma treatment of GO using a mixture of NH3 and Ar as the working gas. When the ratios of NH3:Ar were 1:2, 1:3, and 1:4, the specific capacitances of the GO-P(NH3:Ar = 1:2), GO-P(NH3:Ar = 1:3), and GO-P(NH3:Ar = 1:4) were 124.5, 187.7, and 134.6 F·g−1, respectively, which were 4.7, 7.1, and 5.1 times that of GO at the current density of 1 A·g−1. The capacitance retention of the GO-P(NH3:Ar = 1:3) was 80% when it was cycled 1000 times. The characterization results showed that the NH3 cold plasma could effectively produce N-doped GO and generate more active defects. The N/C ratio and the contents of pyridinic nitrogen and graphitic nitrogen of the GO-P(NH3:Ar = 1:3) were the highest. These were conducive to providing pseudocapacitance and reducing the internal resistance of the electrode. In addition, the ID/IG of the GO-P(NH3:Ar = 1:3) (1.088) was also the highest, indicating the highest number of defects. The results of discharge parameters measurement and in situ optical emission spectroscopy diagnosis of NH3 plasma showed that the discharge is the strongest when the ratio of NH3:Ar was 1:3, thereby the generated nitrogen active species can effectively promote N-doping. The N-doping and abundant defects were the keys to the excellent electrochemical performance of the GO-P(NH3:Ar = 1:3). NH3 cold plasma is a simple and rapid method to prepare N-doped GO and regulate the N-doping to prepare high-performance supercapacitors.
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Journal of Energy Chemistry
·
2021
·
IF 9.676
Mengqi Zhou,Guoqiang Sun,Shuang-Quan Zang
The society’s urgent demand for environmentally friendly, safe and low-cost energy storage devices has promoted the research of aqueous zinc-ion batteries. However, the uneven deposition of Zn ions on anodes will lead to the growth of the dendrite and reduce the Coulombic efficiency as well as the lifespan of the devices. Herein, we construct an O,N-dual functionalized carbon cloth current collector via a simple hydrothermal strategy, in which the oxygen-containing functional groups and the N heteroatoms can regulate the transmission and deposition of Zn ions, respectively. The proposed synergistic strategy ensures the uniform distribution of Zn ions on the surface of the Zn anode and inhibits the formation of dendrites. The symmetric cell based on the O,N-dual doped carbon cloth presents superior cycling stability (318 h) with a low voltage hysteresis (11.2 mV) at an areal capacity of 1 mAh cm −2 (20% depth of diacharge). Meanwhile, the appreciably low overpotential (16 mV) and high Columbic efficiency (98.2%) also demonstrate that the O,N-dual functionalized carbon cloth can be worked as a promising host for Zn ions deposition.
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ANALYTICA CHIMICA ACTA
·
2020
·
IF 5.977
Ruizhi Tang,Yang Yu,Jing Dong,Yating Yao,Shujuan Ma,Junjie Ou,Mingliang Ye
In bottom-up strategy, specific enrichment of glycopeptides and phosphopeptides from complicated biological samples is a prerequisite for efficient identifying glycosylation and phosphorylation by mass spectrometry . Although there were a plethora of materials used as either hydrophilic interaction liquid chromatography (HILIC) or immobilized metal affinity chromatography (IMAC) adsorbents, even several bifunctional materials for simultaneous enrichment of glycopeptides and phosphopeptides, most of them are not easily commercialized as many other well-performing adsorbents due to the complicated preparation process. In our case, a one-step modification strategy was developed to prepare bifunctional adsorbents for HILIC and IMAC, employing O -phospho- l -serine as the modifier and poly(GMA- co -EDMA) microspheres, a kind of macroporous adsorption resin (MAR) with epoxy groups , as the matrix. The MARs were directly modified with O -phospho- l -serine under facile condition for HILIC strategy and further chelated with Ti 4+ for IMAC strategy. A total of 522 unique N -glycopeptides and 442 unique N -glycosylation sites mapped to 275 N -glycoproteins was identified from HeLa cell proteins, showing excellent enrichment efficiency in HILIC. Additionally, 3141 unique phosphopeptides were unambiguously identified from 200 μg of digest of HeLa cell proteins, demonstrating great enrichment efficiency in IMAC. Moreover, these materials have been successfully applied in the analysis of multiple biological samples including human serum and milk, demonstrating their feasibility for real sample applications and potential business value.
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JOURNAL OF PHYSICS D-APPLIED PHYSICS
·
2019
·Vol. 52
·期 29
·295502
·
IF 2.829
Binbin Qian,Chaodeng Liu,Junmin Xu,Qingqing Sun,Huige Yang,Wentao Liu,Li Zhang,Takeo Minari,Xuying Liu,Jinzhou Chen
Three-dimensional (3D) nitrogen-doped graphene frameworks contributing to high-efficiency and high-stability Li-S batteries have received wide interest in energy storage fields. Herein, a 3D nitrogen-doped graphene composite framework was prepared with spatial dendritic triamines as crosslinking interconnectors, and subsequently employed for Li-S batteries with high efficiency and stability. The nanoscale spatial network of triamine-bonded graphene as molecular spacers can enlarge the interlayer spacing and change surface topography, which allows the nanocomposites to inhibit phase separation and thus capture and homogeneously store well-dispersed sulfur nanocrystals at a high capacity exceeding 70%, even by a solution process. In our work, the composite of S@GO-TAPA as the cathode material delivers the highest initial discharge capacity of 965 mAh g−1. Besides that, an average coulombic efficiency of 91% is achieved after more than 100 cycles and 66.5% of the capacity remains, even after 100 cycles at 0.2 °C. The results suggest that the shuttle effect is remarkably suppressed. Therefore, the design strategy for cathode media is promising for fully solution-processing energy storage devices with printing, coating and spraying techniques.
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JOURNAL OF THE EUROPEAN CERAMIC SOCIETY
·
2022
·
IF 6.364
Adeel Abbas,Zhuoming Xu,Mohammad Nisar,Delong Li,Fu Li,Zhuanghao Zheng,Guangxing Liang,Ping Fan,Yue-Xing Chen
SnSe is a very strong anisotropic material; sometimes, strong anisotropy is unenviable for producing parts of thermoelectric (TE) devices. In order to study the efficient preparation of high-performance n-type polycrystalline SnSe with weak anisotropy, in this work, we combine mechanical alloying at 450 RPM for 10 h and spark plasma sintering at 773 K under 50 MPa pressure for the preparation of polycrystalline SnSe 0.95- x I x ( x = 0,0.01,0.02,0.03) samples, and investigate the TE properties. The prepared samples show very weak anisotropy. With iodine doping, increased carrier concentration is observed, in agreement with DFT calculations. A peak ZT ≈ 1.02 at 723 K is observed with I-doping of x = 0.02, which is about 225% higher than that of undoped sample with ZT ≈ 0.31 at 723 K in parallel direction, mainly attributed to the enhanced power factor and about 56% reduced thermal conductivity from 0.68 Wm −1 K −1 to 0.30 Wm −1 K −1 . TE properties in both directions are not much different, and the ratios of electrical and thermal conductivities in both directions are very close to unity.
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Journal of Cleaner Production
·
2022
·
IF 11.072
Shunan Yin,Jinxian Zhao,Shiping Wu,Xuhui Wang,Yanhong Quan,Jun Ren
Electrochemical reduction of CO 2 to valuable chemicals using electricity from renewable sources is a promising approach to realize the carbon cycle. Here, a novel bimetallic nitrogen-doped carbon catalyst (M-N-C, where M denotes the metal) CoCu–N–C electrocatalyst has been synthesized by pyrolyzing a copper-doped cobalt(II) acetate–phenanthroline complex formed from the metal acetates and 1,10-phenanthroline dissolved in ethanol. The optimal CoCu–N–C catalyst with molar ratio of Cu/(Co + Cu) = 0.15 displayed superior performance, enabling a faradaic efficiency of CO production of 76.5% at an overpotential of 0.57 V as well as an increased CO current density of 8.48 mA cm −2 at −0.98 V versus reversible hydrogen electrode (far superior than the Co–N–C of 4.20 mA cm −2 and Cu–N–C of 0.07 mA cm −2 ) and a decreased charge-transfer resistance compared with Co–N–C and Cu–N–C catalysts. The addition of Cu, which serves as a structure promoter to improve the dispersion of Co, thereby providing sufficient Co-N x active sites for the electrochemical CO 2 reduction reaction (CRR). Moreover, doping Cu changes the electronic environment around Co slightly and promotes the charge transfer capability so that reduces the energy barrier of potential-limiting energy, thereby improving the CRR performance of catalyst.
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JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2020
·
IF 3.807
Xiuxian He,Zheng Tang,LianLian Gao,Fangyuan Wang,Jinping Zhao,Zhichao Miao,Xiaozhong Wu,Jin Zhou,Yang Su,Shuping Zhuo
Engineering graphene with efficient ion and electron transport properties is vital for development of high performance, next generation energy storage devices. The protocols generally involve pore generation and doping of graphene with the heteroatoms. Herein we report the realization of pore generation, control, and N-doping of graphene in one single process using reduced metal salt as etching agent and environment friendly N 2 gas as doping agent. Furthermore, we found the porous structure (pore size and density), the dopant bonding configuration and doping amount can be controlled by change the metal salt and nitrogen source, which allows us to investigate the influence of pore and N-doping structure of porous graphene (PG) in their supercapacitor performance . Specifically, the N-doping, PG prepared by Ni salt (PG-Ni) shows the smaller pore size (average pore size of ~20–30 nm) and larger pore density. PG-Ni exhibits high specific capacitance of 575 F/g along with the energy density of 51.2 Wh/kg at 0.5 A/g current density and also shows good rate, cycling performances. Considering the excellent performance, ease of the process, and pore structure controllability, we believe the method provides a new route for developing graphene based high performance supercapacitors.
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ACS Sustainable Chemistry & Engineering
·
2021
·
IF 8.198
Shuang Xu,Xiaopo Niu,Gang Yuan,Zheyuan Wang,Shuaikang Zhu,Xiaoxue Li,Yunxi Han,Rong Zhao,Qingfa Wang
Electrocatalytic synthesis of valuable biofuels and chemicals from biomass-derived acids is a promising approach, but selectively producing deoxygenated hydrocarbons is still a great challenge. In this work, we investigated selective electrochemical decarboxylation of n-octanoic acid to produce hydrocarbons (n-tetradecane, n-heptane, and n-heptene) in a single electrolytic cell at room temperature. Pt nanoparticles with different morphologies (nanospheres, nanoflowers, and nanothorns) and further Pt nanothorns with different plane distributions on carbon fiber paper (CFP) were fabricated by a controllable electrodeposition method. The results proved that the Pt(311) plane has the best selectivity and intrinsic activity for decarboxylation products, especially for Kolbe hydrocarbons. The Pt(110) plane shows a similar intrinsic activity as the Pt(311) planes. High selectivity (75%), yield (35%), and Faraday efficiency (34%) for hydrocarbons were achieved over the Pt nanothorn (Pt-NT), which were approximately 1.6, 2.3, and 3.3 times that of Pt nanoflowers, Pt nanospheres, and Pt/C, respectively. The high electrocatalytic activity of Pt nanothorns was attributed to its high electrochemically active surface area (ECSA) and enhanced intrinsic activity derived from the high level of Pt(311) and Pt(110) planes.
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危险品化学品经营许可证（带存储）