NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 38
·16526-16536
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IF 3.288
Xufeng Bai,Ting Ren,Jingbo Mao,Shenmin Li,Jingmei Yin,Jinxia Zhou
Cellulose-derived levulinic acid (LA) can be converted into gamma-valerolactone (GVL), a sustainable platform chemical for the production of bio-based chemicals. However, LA as an organic acid causes severe metal leaching during the heterogeneous hydrogenation of LA to GVL, especially in the presence of water. Various endeavors for preventing metal leaching have focused more on the process and less on the intrinsic nature of catalysts. The aim of this work is to derive a novel metal-leaching-resistant catalyst for the aqueous-phase hydrogenation of LA into GVL by using a nanocomposite containing three components, Ag, ZrO2, and graphene oxide (GO). The AgZrO2GO catalyst without pre-reduction treatment resulted in complete conversion of LA and approximately 100 mol% selectivity to GVL in the aqueous reaction, and metal leaching from the catalyst was completely eliminated. The relationship between the catalytic performance and the distinct physicochemical properties of the catalyst was extensively discussed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
·
IF 7.489
Jianwei Feng,Ling Liu,Qinghan Meng
In this paper, we designed and prepared a novel metal organic framework (MOF)/holey graphene (HG) composites as electrode materials for electrochemistry and capacitive deionization (CDI). The MOF nanoparticles were attached to the surface of the HG sheets to form layered porous structure, which promoted the transport of ions and electrons in the electrode/electrolyte interfaces. Additionally, the synergistic effect of these composite electrodes, which combined pseudocapacitance performance of MOF and the high conductivity of graphene, contributed to enhancing the performance of electrochemistry and CDI. The MOF/HG-2 exhibited high capacitances of 526 F g −1 at current rates of 0.1 A g −1 , low charge transfer resistance of 0.53 Ω, and excellent cycling stability (retention of about 90.3% after 5000 cycles at 2 A g −1 ). As electrode materials for CDI, the MOF/HG-2 displayed a remarkable electrosorption capacity of 39.6 mg g −1 with initial salt concentration of 800 mg L −1 , and there was no obvious attenuation after 20 CDI regeneration cycles. These results confirmed that MOF/HG was a promising electrode material for the actual application of CDI.
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Frontiers in Chemistry
·
2020
·
IF 3.693
Liu Yali,Zhou Mingyue,Jin Chen,Zeng Jinxiang,Huang Chao,Song Qiuye,Song Yonggui
In this work, a covalent-organic framework with high carbon and nitrogen content microstructures (named COF-LZU1), assisted by 3D nitrogen-containing kenaf stem composites (represented as COF-LZU1/3D-KSCs), was constructed. Moreover, it was utilized for immobilizing acetylcholinesterase (AChE) for identifying trichlorfon, a commonly applied organophosphorus (OP) pesticide. The development of COF-LZU1/3D-KSC was affirmed by SEM, PXRD, and EDXS. The findings confirmed that COF-LZU1 microstructures were uniformly developed on 3D-KSC holes using a one-step synthesis approach, which can substantially enhance the effective surface area. Also, the COF-LZU1/3D-KSC composite contains not only the nitrogen element in COF-LZU1 but also the nitrogen element in 3D-KSC, which will greatly improve the biocompatibility of the material. The AChE/COF-LZU1/3D-KSC integrated electrode was fabricated by directly fixing a large amount of AChE on the composite. At the same time, the integrated electrode had good detection efficiency for trichlorfon. Improved stabilization, a wide-linear-range (0.2–19 ng/mL), and a lower detection limit (0.067 ng/mL) have been displayed by the sensor. Therefore, this sensor can be used as an important platform for the on-site detection of OP residue.
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MATERIALS CHEMISTRY AND PHYSICS
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2020
·
IF 3.408
Tao Guo,Ting Xu,Wentao Xia,Andrew J. Carrier,Li Wang,Xu Zhang
We report herein, double quantum dot composites of graphene oxide and CuO (GOQD-q-CuO), formed by a low-temperature solution process, possess enhanced haloperoxidase (HPO)-like catalytic activity, which catalyze the oxidation of Cl − by H 2 O 2 to generate reactive chlorine species (RCS). A sensitive and selective colorimetric sensor was then developed via the oxidation of 3,3ʹ,5,5ʹ-tetramethylbenzidine (TMB) by the GOQD-q-CuO catalytic system through the generation of RCS for H 2 O 2 and glucose detection, with detection limits of 0.5 and 2.5 μM and linear ranges between 2.5–200 and 5–400 μM, respectively. This sensor was further applied to glucose detection in clinical serum samples showing no significant differences with the hexokinase method. Additionally, we demonstrate that the GOQD modulates the catalytic activity of q-CuO by reversing its zeta potential , producing an overall negatively charged surface, therefore GOQD-q-CuO has much higher affinity than CuO to the positively charged chromogenic substrate TMB, yielding higher HPO-like activity. Moreover, the presence of Cl − accelerates electron transfer to facilitate Cu 2+ reduction to Cu + on the GOQD-q-CuO surface, speeding up the overall catalytic reaction for the RCS generation, therefore, higher detection sensitivity was achieved.
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RSC Advances
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2020
·Vol. 10
·期 71
·43762-43772
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IF 3.119
Qianqian Zhao,Guo Feng,Feng Jiang,Shanfang Lan,Junhua Chen,Mengting Liu,Zuzhi Huang,Jianmin Liu,Qing Hu,Weihui Jiang
Fe2TiO5/C photocatalysts were synthesized by a solid-state reaction method (Fe2TiO5/C(S)) and nonhydrolytic sol–gel (NHSG) method (Fe2TiO5/C(N)), where C was introduced by external carbon and in situ carbon sources, respectively. The Fe2TiO5/C(N) photocatalyst with in situ carbon has much better photocatalytic degradation efficiency than that of Fe2TiO5/C(S) synthesized by doping external carbon. The superiorities of in situ carbon were demonstrated by SEM, EDS, BET and photoelectrochemical analysis. Compared with Fe2TiO5/C(S) using external carbon as a carbon source, Fe2TiO5/C(N) with in situ carbon exhibits more uniform elemental distribution, much larger surface area, higher photocurrent density and lower resistivity of interfacial charge transfer. The results show that the introduction of in situ carbon via the NHSG method more easily promotes the separation of photogenerated electron–hole pairs, owing to the uniformity of the carbon element, thereby improving the photocatalytic activity of the photocatalyst.
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Analytical Methods
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2020
·Vol. 13
·期 5
·672-684
·
IF 2.596
Xiao-Chun Ma,Zong-Qin Ma,Meng-Xin Zhao,Ying-Hui Wang,Yuan Peng,Xin Guo,Fang-Huan Wang,Zhe Meng,Hao-Bo Zheng
A novel magnetic molybdenum disulfide@graphene (Fe3O4/MoS2@G) nanocomposite with amphiphilic properties was prepared via a co-mixing solvothermal method. To demonstrate the feasibility of Fe3O4/MoS2@G as a sorbent during sample preparation, it was employed for the magnetic solid phase extraction (MSPE) of ten pyrethroids, three triazoles and two acaricide pyridaben and picoxystrobin in an emulsified aqueous solution. Dichloromethane was used as the extractant to form an emulsified aqueous solution. Subsequently, the Fe3O4/MoS2@G sorbent with amphiphilic properties was used to retrieve 15 wide polarity insecticides from dichloromethane via MSPE. The proposed method has the advantage of being applicable to different polar pesticides, strengthening the capacity of enrichment and purification of target analytes. The π–π interaction between the hydrophilic and hydrophobic moieties of Fe3O4/MoS2@G and the aromatic rings of target analytes were responsible for the efficient sorption. Thus, a reliable, convenient, and efficient method for the analysis of 15 insecticides with wide polarity in wolfberry samples was established by coupling Fe3O4/MoS2@G nanocomposite MSPE with gas chromatography-mass spectrometry (GC-MS) analysis. The obtained linearity of this method was in the range from 1 to 5000 ng mL−1 for 15 analytes, with determination coefficients (R2) ≥0.9907. The limit of detection (LOD) for 15 insecticides was in the range from 0.1 to 5.0 ng g−1. The recoveries of 15 insecticides from spiked wolfberry samples were in the range from 71.41% to 110.53%, and RSD was less than 14.8%.
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CHEMICAL ENGINEERING JOURNAL
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2020
·
IF 10.652
Yanpei Li,Lei Shi,Xingpeng Gao,Jingyi Wang,Yingying Hu,Xiangwei Wu,Zhaoyin Wen
The hierarchical nickel chloride/reduced graphene oxide (NiCl 2 -rGO) aerogels are synthesized via a facile hydrothermal and freeze-drying methods using low-cost nickel chloride hexahydrate (NiCl 2 ·6H 2 O) as raw material. The NiCl 2 -rGO hybrid aerogel structure enables the uniform distribution of lamellar NiCl 2 on the three-dimensional (3D) cross-linked conductive graphene sheets. When employed as cathode for sodium-nickel chloride (Na-NiCl 2 ) batteries, the as-obtained NiCl 2 -rGO aerogels exhibit excellent electrochemical performance with high reversible capacities (116 mAh g −1 after 50 cycles, 128 mAh g −1 in a fixed capacity window (20%–80% state of charge (SOC)) after 50 cycles), and a ultra-low polarization (0.05 V in the fixed capacity window). The outstanding performance of NiCl 2 -rGO aerogels can be attributed to the excellent conductivity of graphene. Moreover, the strong contact between NiCl 2 and graphene sheets can effectively promote the transfer of electrons. Compared with traditional tubular Na-NiCl 2 batteries, the molar ratio of Ni/NaCl of NiCl 2 -rGO aerogels can be decreased from 1.8 to the stoichiometric ratio (0.5). To the best of our knowledge, this work paves a perspective way for the first time to develop charged-state NiCl 2 -based cathodes with splendid performance for Na-NiCl 2 batteries.
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Energy & Environmental Science
·
2020
·Vol. 14
·期 1
·382-395
·
IF 30.289
Wei Liu,Zidong Chen,Zheng Zhang,Pingxian Jiang,Yungui Chen,Eunsu Paek,Yixian Wang,David Mitlin
Sodium metal battery (SMB, NMB) anodes can become dendritic due to an electrochemically unstable native Na-based solid electrolyte interphase (SEI). Herein Li-ion activated tin sulfide graphene nanocomposite membrane (A-SnS–G) is employed as an artificial SEI layer, allowing cyclability of record-thin 100 μm Na metal foils. The thin Na metal is prepared by a self-designed metallurgical rolling protocol. A-SnS–G is initially placed onto the polypropylene (PP) separator but becomes in situ transferred onto the Na metal surface. Symmetric metal cells protected by A-SnS–G achieve low-overpotential extended high-rate cycling in a standard carbonate electrolyte (EC : DEC = 1 : 1, 5% FEC). Accumulated capacity of 1000 mA h cm−2 is obtained after 500 cycles at 4 mA cm−2, with accumulated capacity-to-foil capacity (A/F) ratio of 90.9. This is among the most favorable cycle life, accumulated capacity, and anode utilization combinations reported. Protection by non-activated SnS–G membrane yields significantly worse cycling, albeit still superior to the baseline unprotected sodium. Post-mortem and dedicated light optical analysis indicate that metal swelling, dendrite growth and dead metal formation is extensive for the unprotected sample, but is suppressed with A-SnS–G. Per XPS, post-100 cycles near-surface structure of A-SnS–G is rich in metallic Sn alloys and inorganic carbonate salts. Even after 300 cycles, Li-based SEI components ROCO2-Li, Li2CO3 and LiF are detected with A-SnS–G. As a proof of principle, an SMB with a high mass loading (6 mg cm−2) NVP cathode and a A-SnS–G protected anode delivered extended cyclability, achieving 74 mA h g−1 after 400 cycles at 0.4C.
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RENEWABLE ENERGY
·
2020
·
IF 6.274
Ting Zhang,Tuodi Zhang,Jing Zhang,Deyi Zhang,Pengran Guo,Hongxia Li,Chunlei Li,Yi Wang
The large-scale commercial application of phase change materials (PCMs) was seriously limited by the leakage, poor heat storage capacity and slow thermal response behavior. To address these issues, stearic acid/graphene oxide-attapulgite aerogel (SA/HGA-ATP) shape-stabilized PCMs were fabricated via hydrothermal method . The morphology, structural characteristics, thermal properties were determined and the effects of ATP percentage on the thermal properties of confined SA were studied synchronously. The nanofibers of ATP intercalated among GO sheets via grafting modification and formed fiber-bridging 3D-network. Due to the enhanced loading interspaces and suppressed volumetric shrinkage of hybrid matrix, SA/HGA-ATP exhibited excellent thermal energy storage capacity (190.9 J g −1 ) and ultra-high SA contents (approx. 98 wt%) without leakage. The intercalated nanofibers sheltered the oxygen-containing groups of matrices, leading to the promotion of thermal energy storage performance with increase of ATP contents. Besides, the as-prepared PCMs displayed outstanding thermal response behavior because the interconnected and fiber-bridged matrices provided continuous thermal transfer pathway. Due to the protection of matrix, the composite PCMs also exhibited superior structure stability and incomparable thermal energy storage/release reliability. Considering the outstanding thermal-physical properties and low-cost of ATP, the SA/HGA-ATP has the potential to be applied in the fields of thermal energy storage, conversion and utilization.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Qi Zhao,Wenxin Gou,Xueting Zhang,Mengyuan Zhang,Yanru Bu,Lijun Wang,Lei Hu,Wenli Yao,Zhengquan Yan
To improve the selectivity and sensitivity for naked-eye detection of toxic Hg 2+ , water-soluble Ag 2 S nanoparticle stabilized by graphene oxide (Ag 2 S@GO) was identified by virtue of the high catalytic activity of nano Ag 2 S and the excellent physicochemical property of graphene oxide. After its structure and spectral performance were characterized and investigated, it was noted that the proposed Ag 2 S@GO possesses outstanding Hg 2+ -activated oxidase-like activity to oxidize the chromogenic substrate of 3,3′,5,5′,-tramethylbenzidine (TMB) with an obvious hyperchromic effect from colorless to blue in the presence of Hg 2+ exclusively. Under the optimized conditions, the Ag 2 S@GO+TMB system was successfully applied for naked-eye detection of heavy metal Hg 2+ in real environmental samples, with a nmol·L −1 -level detection limit of 9.8 × 10 –9 mol/L, an accurate recovery among 97.0–101.8% and a low standard deviation less than 3.3%. The Hg 2+ -activated oxidase-like activity of Ag 2 S@GO and its exclusive recognition mechanism to toxic Hg 2+ were also proposed.
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HIGH PERFORMANCE POLYMERS
·
2020
·
IF 1.568
Hai-Hui Liu,Meng-Qi Zhang,Zi-Han Tian,Peng-Fei Liu,Yan-Xin Liu,Xing-Xiang Zhang
Freestanding poly(3,4-ethylenedioxythiophene) (PEDOT) nanowires (NWs) were synthesized using a facile, self-assembled, micellar soft-template method. Thermoelectric properties of the PEDOT NWs under different reaction conditions were measured, and optimal experimental conditions were confirmed. To obtain preferential thermoelectric performance, PEDOT NWs/graphene composite films with various graphene mass fractions were fabricated. The maximum power factor of the hybrids was observed to reach 42.0 μWm−1K−2 with 3 wt% graphene loading, corresponding to a 200% improvement compared with pure PEDOT NWs. The thermoelectric devices were investigated using the PEDOT NWs/graphene hybrids as a p-type leg and PEDOT NWs/nitrogen-doped graphene as an n-type leg. The device, in series, shows a preferable cooling effect with an approximate temperature decrease of 0.5°C after energization. Our work provides a novel means of fabricating n-type PEDOT hybrids and promotes their practical applications as thermoelectric coolers. These findings indicate a new means of developing high-performance, flexible, organic thermoelectric materials and devices.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Huizhen Deng,Juanjuan Yin,Jinming Ma,Jingxin Zhou,Lexin Zhang,Lili Gao,Tifeng Jiao
A novel catalyst composed of Ag 3 PO 4 bridged by Ni/Ti LDH-graphene heterojunction structure was successfully prepared by a simple in-situ deposition method, which has excellent catalytic performance for 4-NP and 2-NA. Various characterizations to the samples such as XRD, SEM, TEM, STEM-EDS, XPS, TG–DSC, and UV–vis DRS were adopted. Because the ternary structure is mixed with each other to form more heterojunctions and higher specific surface area, the ternary composite Ag 3 PO 4 /Ni-Ti LDH/GO has excellent catalytic and cycle performance. Compared to the precursors Ag 3 PO 4 /GO and Ni-Ti LDH/GO, the finally as-obtained nanocomposite Ag 3 PO 4 /Ni-Ti LDH/GO degraded 4-NP and 2-NA solutions represented more dominant degradation efficiency. In addition, the pseudo-first-order rate constants of the composite catalyst for 4-NP and 2-NA are 0.178 min −1 and 0.089 min −1 , respectively. The complex and irregular surfaces of Ni-Ti LDH/GO provided an ideal carrier with abundant active sites for in-situ depositing and stabilizing of Ag 3 PO 4 NPs, formed the Ag 3 PO 4 /Ni-Ti LDH/GO hybrid possessed an acceptable catalytic performance on the degradation of azo dyes, which could be applied in the efficient treatment of wastewater from industries.
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