ELECTROCHIMICA ACTA
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2022
·
IF 7.336
Shiliu Yang,Quanzhou Yin,Jiabiao Lian,Guochun Li,Yijun Wei,Qiyong Zhu
Polyaniline (PANi) has brought new enthusiasm in the field of aqueous Zn-ion batteries due to the unique nature of high conductivity, excellent structural flexibility, and fast ions de-/intercalation ability. However, the naked and densified PANi usually suffers from capacity fade and limited rate performance owing to the deprotonation of the polymer and imbalanced electron-ion transmission. Herein, a HCl-doped porous PANi electrode was prepared by electrodepositing the aniline monomer onto a porous carbon cloth (PCC), which plays an important role in elevating the loading mass and inducing porous structure of the PANi, thus enhancing the mass energy density and ions diffusion coefficient of the electrode; On the other hand, the HCl-doping could facilitate the charge delocalization and increase the conductivity of the PANi. Besides, a convertible behavior of the energy storage sites during charging-discharging processes was firstly observed for PANi, which should be responsible for the high-rate and cycling performance of the Zn-ion batteries, there is very small capacity decay from 170 mAh g −1 at 1 A g −1 to 161 mAh g −1 at 10 A g −1 , and 87 % of the initial the capacity can maintain after 2000 cycles at 5 A g −1 . Furthermore, the quasi-solid-state Zn-ion battery can also display superior performance, showing potential application of the PCC@PANi for wearable devices
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JOURNAL OF MOLECULAR LIQUIDS
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2022
·
IF 6.633
Congcong Chen,Ying Xie,Lingyi Jia,Yong Zhang
Efficient capture of Th(IV) from aqueous solution is of importance to both solve the radioactive pollution for environmental safety and provide clean energy for sustainable development. However, it still faces huge challenge. In this study, eucalyptus leaf extract was applied as template agent to fabricate Zn/Al-bimetallic layered double oxides (ZnAlLDO), providing more active sites for Th(IV) removal. The removal process of Th(IV) onto ZnAlLDO could reach equilibrium within 5 min and the maximum removal capacity calculated from the Langmuir model was 1153.71 mg g −1 at pH = 4.0 and 298 K. Over 97 % Th(IV) could be removed by ZnAlLDO during the dynamic adsorption process and the removal efficiency still remained at a high level (85 %) after 5 cycles. The Th(IV) removal process on ZnAlLDO was ascribed to electrostatic attraction, complexation and ion exchange. It could be believed that the ZnAlLDO with large removal capacity (1155.5 mg g −1 ), fast equilibrium time (5 min) and easy desorption (91.76 %) with high recovery (85 %) might be a promising adsorbent for the separation of Th(IV).
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FUEL
·
2023
·
IF 7.4
Xiao-Yan Zhao,Xue-Yu Ren,Yan-Jun Wang,Jing-Pei Cao,Zi-Meng He,Nai-Yu Yao,Hong-Cun Bai,Hou-Luo Cong
Direct conversion of lignite into light aromatics via catalytic fast pyrolysis is a great challenge because of severe catalyst deactivation and low aromatics yield. The tandem catalysis (1Zn@MCM-41 and ZSM-5) system was employed to promote the conversion of thermally-derived volatiles of lignite into aromatics at 600 °C. The mesoporous Zn-incorporated MCM-41 (xZn@MCM-41) with different doping amount of Zn was prepared with a one-pot hydrothermal procedure. The structure and the dispersion of Zn species of 1Zn@MCM-41 were systematically studied with XRD, SEM, BET, NH 3 -TPD and so on. The presence of 1Zn@MCM-41 significantly expands the lifetime of the microporous ZSM-5. Meanwhile, the yield of aromatics, especially benzene, is also increased to some extent. The content of the long-chain hydrocarbons and the phenolic compounds are decreased significantly after being cracked by the mesoporous 1Zn@MCM-41. More small molecules are able to contact with the active sites located in the micropores of ZSM-5 with the presence of Zn@MCM-41. In addition, the ZSM-5 in the tandem catalysts system presents an excellent stability. Therefore, this meso -microporous tandem catalysis system promotes the preferential cracking of macromolecular compounds, the cracked small molecules generated from which then contact with ZSM-5 to produce aromatics. This work provides a new perspective for the gradient catalyzing lignite-derived volatiles over a tandem catalysis system.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Zihao Chen,Senjie Dong,Minghui Wang,Zunpeng Hu,Huiling Chen,Ye Han,Ding Yuan
Constructing three-dimensional (3D) hierarchical heterostructures is an appealing but challenging strategy to improve the performance of catalysts for electrical energy devices. Here, an efficient and robust flexible self-supporting catalyst, interface coupling of ultrathin CoFe-LDH nanosheets and Co3O4 nanowire arrays on the carbon cloth (CC/Co3O4@CoFe-LDH), was proposed for boosting oxygen evolution reaction (OER) in rechargeable liquid/solid Zn–air batteries (ZABs). The strong interfacial interaction between the CoFe-LDH and Co3O4 heterostructures stimulated the charge redistribution in their coupling regions, which improved the electron conductivity and optimized the adsorption free energy of OER intermediates, ultimately boosting the intrinsic OER performance. Besides, the 3D hierarchical nanoarray structure facilitated the exposure of catalytically active centers and rapid electron/mass transfer during the OER process. As such, the CC/Co3O4@CoFe-LDH catalyst achieved excellent OER catalytic activity in alkaline medium, with a small overpotential of 237 mV at 10 mA cm–2, a low Tafel slope of 35.43 mV dec–1, and long-term durability of up to 48 h, significantly outperforming the commercial RuO2 catalyst. More impressively, the liquid and flexible solid-state ZABs assembled by the CC/Co3O4@CoFe-LDH hybrid catalyst as the OER catalyst presented a stable open circuit voltage, large power density, superb cycling life, and satisfactory flexibility, indicating great potential applications in energy technology. This work provides a good guidance for the development of advanced electrocatalysts with heterostructures and an in-depth understanding of electronic modulation at the heterogeneous interface.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Hao Xu,Lihui Xiao,Peixia Yang,Xiangyu Lu,Lilai Liu,Dan Wang,Jinqiu Zhang,Maozhong An
Zeolitic imidazole framework (ZIF)-derived iron–nitrogen-carbon (Fe N C) materials are expected to be high-efficiency catalysts for oxygen reduction reaction (ORR). However, increasing the density of active sites while avoiding metal accumulation still faces significant challenges. Herein, solvent environment engineering is used to synthesize the Fe N C containing dense Fe-N x moieties by adjusting the solvent during the ZIF precursor synthesis process. Compared with methanol and water/methanol, the aqueous media can provide a more moderate Fe content for the ZIF precursor, which facilitates the construction of high-density Fe-N x sites and prevent the appearance of iron-based nanoparticles during pyrolysis. Therefore, the Fe N C(C) nanocubes synthesized in an aqueous media have the highest single atom Fe loading (0.6 at%) among the prepared samples, which presents excellent oxygen reduction properties and durability under alkaline and acidic conditions. The advantage of Fe N C(C) is proven in Zn-air batteries, with outstanding performance and long-term stability.
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CHEMICAL ENGINEERING JOURNAL
·
2022
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IF 16.744
Zhaopeng Xia,Jiajun Pan,Hao Chen,Nanping Deng,Chao Yang,Xiaochen Liu,Yong Liu,Liwei Wu
Many researches are devoted to design the wearable fibrous energy storage devices with miniaturization in order to satisfy the large demand of power for portable wearable electronics. As a kind of flexible battery, one-dimensional yarn-like nickel-zinc (Ni-Zn) battery has a lot of disadvantages such as low energy density and poor power density. Significantly, metal–organic framework (MOF) material provides an opportunity to solve the preceding shortcomings due to its porous structure, excellent specific surface area and multi-functionalization. In this study, the nickel cobalt layered double hydroxides (NiCo LDHs) with triangular micro sheet array and nano sheet structure is designed and prepared on silver coated nylon fibers (SCNF) as the flexibly fibrous Ni-Zn battery cathodes (SCNF@Ni@MOF@NiCo LDHs yarn electrode), which have high specific surface area and super structure stability even during bending of the yarn. Therefore, the cathodes have abundant active sites, excellent electron conduction and fast ion diffusion. The assembled aqueous Ni-Zn battery is featured with suitable capacitance (342 mAh/g at 7.6 A/g), appropriate energy density (572.5 Wh/g at 2.59 W g −1 ) and superior stability (55 % after 5000 cycles). In addition, the obtained one-dimensional yarn-like Ni-Zn battery has excellent flexibility and high capacity retention (90 % after 1000 bends and over 80 % after different deformation ways such as bend, squeeze and twist). These fascinating results demonstrate that the SCNF@Ni@MOF@NiCo LDHs yarn electrode have great application potential in wearable energy storage devices.
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Small Methods
·
2022
·Vol. 6
·期 12
·2201142
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IF 15.367
Ce Qiu,Jia Liu,Hanghui Liu,Xiaohui Zhu,Liang Xue,Shuang Li,Mingzhu Ni,Yang Zhao,Tong Wang,Serguei V. Savilov,Sergey M. Aldoshin,Hui Xia
Although birnessite-type manganese dioxide (δ-MnO 2 ) with a large interlayer spacing (≈7 Å) is a promising cathode candidate for aqueous Zn/MnO 2 batteries, the poor structural stability associated with Zn 2+ intercalation/deintercalation limits its further practical application. Herein, δ-MnO 2 ultrathin nanosheets are coupled with reduced graphene oxide (rGO) via van der Waals (vdW) self-assembly in a vacuum freeze-drying process. It is interesting to find that the presence of vdW interaction between δ-MnO 2 and rGO can effectively suppress the layered-to-spinel phase transition in δ-MnO 2 during cycling. As a result, the coupled δ-MnO 2 /rGO hybrid cathode with a sandwich-like heterostructure exhibits remarkable cycle performance with 80.1% capacity retained after 3000 cycles at 2.0 A g −1 . The first principle calculations demonstrate that the strong interfacial interaction between δ-MnO 2 and rGO results in improved electron transfer and strengthened layered structure for δ-MnO 2 . This work establishes a viable strategy to mitigate the adverse layered-to-spinel phase transition in layered manganese oxide in aqueous energy storage systems.
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Energy Storage Materials
·
2022
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IF 20.831
Huan Yang,Shuai Gao,Dewei Rao,Xiaohong Yan
Developing cost-effective and high-efficient bifunctional electrocatalyst for both oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is essential for rechargeable Zn-air battery application. However, achieving high-active dual sites for bifunctional oxygen electrocatalysis in a single catalyst, as well as determining the decisive active sites for OER and ORR to explore the synergistically catalytic mechanism remain challenges. Herein, we propose a catalyst consisting of high-purity pyrrole nitrogen anchored cobalt single-atom (CoN 4 ) and adjacent metallic cobalt sites (Co p @CoNC) for explicit research of dominated active sites. The obtained Co p @CoNC exhibits superior electrocatalytic activity with a small overpotential difference of 0.68 V between OER potential at 10 mA cm −2 and ORR half-wave potential, outperforming commercial noble-metal based catalysts. Electrochemical measurements and theoretical simulations verify the pyrrole-type CoN 4 and adjacent metallic cobalt are separately decisive active sites for ORR and OER activities. Simultaneously, metallic cobalt regulates electron distribution of CoN 4 moiety to improve ORR activity. Importantly, the rechargeable liquid and flexible solid-state Zn-air batteries using Co p @CoNC as air electrode catalysts possess high peak power densities of 188.8 and 121.8 mW cm −2 , respectively. Our findings provide a feasible strategy to design high-performance multifunctional catalysts for rechargeable Zn-air batteries application.
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TRANSACTIONS OF NONFERROUS METALS SOCIETY OF CHINA
·
2022
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IF 3.752
Qian WEI,Liu-yang DONG,Cong-ren YANG,Xue-duan LIU,Fen JIAO,Wen-qing QIN
Lime (CaO) and sodium humate (NaHA) were used as the combined depressant for arsenopyrite pre-treated by CuSO 4 and butyl xanthate. Micro-flotation tests show that the combined depressant CaO and NaHA achieved the selective depression of arsenopyrite. Closed-circuit lab-scale test results indicate that the synergistic effect of CaO+NaHA achieved a satisfactory flotation separation of sphalerite and arsenopyrite, for which the Zn grade and recovery of Zn concentrate were 51.21% and 92.21%, respectively. Contact angle measurements, adsorption amount measurements and X-ray photoelectron spectroscopy analysis indicate that the dissolved calcium species (mainly as Ca 2+ ) were adsorbed on the mineral surfaces, thereby promoting NaHA adsorption. Moreover, the surface of the arsenopyrite absorbed more amount of calcium species and NaHA than that of the sphalerite, thereby accounting for the strong hydrophilic surface of arsenopyrite. The adsorption of NaHA on arsenopyrite was mainly chemical adsorption through its carboxyl groups and Ca atoms, whereas that on sphalerite surface was relatively weak.
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JOURNAL OF THE SCIENCE OF FOOD AND AGRICULTURE
·
2022
·Vol. 102
·期 11
·4714-4723
·
IF 4.125
Ke Cheng,Jianghua Zhang,Shasha Yang,Fawen Yin,Zixuan Li,Ting Wang,Dayong Zhou
BACKGROUND Efficient and sustainable production of structured phospholipids (SPLs) enriched in medium-chain fatty acids (MCFAs) in a heterogeneous manner is crucial for their potential applications in functional foods and drugs. Herein, for the first time, Zn- and Al-incorporated SBA-15 silicas were prepared by the coprecipitation method and further researched for catalytic synthesis of MCFA-enriched SPLs through acidolysis reaction of natural phospholipids with capric or caprylic acid. RESULTS The as-prepared Zn- and Al-incorporated SBA-15 samples exhibited superior catalytic activities under mild experimental conditions (50 °C, 6 h) to commercial homogeneous Lewis acids and benchmark enzymes. Correspondingly, the capric acid and caprylic acid incorporations were respectively achieved up to ~40.25 ± 0.40% (or 35.08 ± 0.09%) and 37.26 ± 0.38% (or 33.02 ± 0.13%) for Zn- (or Al-) incorporated SBA-15 catalyst. Moreover, various methods such as scanning electron microscopy with energy-dispersive X-ray spectrometry, ultraviolet–visible diffuse reflectance spectroscopy and pyridine–Fourier transform infrared spectroscopy were utilized to characterize the two catalysts in order to elucidate the possible structure–performance relationship. Accordingly, the above-mentioned satisfactory results are most probably due to the well-ordered mesostructures and large amounts of active Lewis acid sites existing in the investigated materials. Noticeably, the two catalysts featured good separation and excellent recyclability as well. CONCLUSION The Zn- and Al-incorporated SBA-15 catalysts studied in this work might shed light on novel, sustainable and economic alternatives for effective SPL production to diminish the applications of conventional homogeneous catalysts and biocatalysts in food industries. © 2022 Society of Chemical Industry.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
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IF 6.371
Zhenzhen Wang,Xiaozhuang Zhou,Huihui Jin,Ding Chen,Jiawei Zhu,Rolf Hempelmann,Lei Chen,Shichun Mu
Developing bifunctional ORR&OER electrocatalysts with high activity and stability is challenging for practical application of rechargeable Zinc air batteries. Herein, an ionic liquid strategy is proposed for construction of FeCo alloys encapsulated in nitrogen-doped carbon as bifunctional electrocatalyst for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). By taking advantages of the unique properties such as solvent effect and low volatility, ionic liquid serves as solvent to disperse metal ions in the precursor preparation and nitrogen-containing carbon source during pyrolysis. The FeCo alloy nanoparticles encapsulated in the N-doped carbon matrix show a homogeneous distribution with average sizes of 50–100 nm. Such a core-shell structure endows the catalyst with both high ORR and OER activity and robust stability in alkaline environments. Especially, the half-wave potential (E 1/2 ) for ORR is 0.86 V and the overpotential (E over ) for OER to reach the 10 mA·cm −2 current density is only 280 mV. Furthermore, the obtained bifunctional electrocatalyst also displays high efficiency and great durability when applied in the rechargeable Zn-air battery. The specific capacity and energy density at the discharge current density of 10 mA·cm −2 reach up to 741.5 mAh·g −1 and 830.1 Wh kg −1 , respectively. It’s envisioned that this ultra-facile method would be applicable to synthesize highly efficient catalysts for other energy conversion systems.
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LANGMUIR
·
2022
·
IF 4.331
Xiaoting Cao,Ruili Song,Xiaoshuang Zhou,Xi Wang,Xu Dong,Ningyi Yuan,Jianning Ding
Electrocatalysts with high cost-effectiveness for the oxygen reduction reaction (ORR) are essential for fuel cells (FC) and Zn-Air batteries (ZAB), which need highly active sites and suitable carbon substrates to accelerate the charge transfer kinetics. Herein, a simple and extensible method using ball milling and space-confinement pyrolysis is reported to prepare a series of transition metals and N-C catalysts (M-NLPC), which possess three-dimensional porous carbon substrates and dense active sites for efficient ORR. M-NLPC catalysts (especially Fe-NLPC) exhibit outstanding ORR activity with a half-wave potential (E1/2, 0.88 V) in an alkaline medium, high stability, and strong methanol resistance. The M-N4 sites are proven to be the active centers in M-NLPC by theoretical calculation, and methanol molecules are more likely to desorb than react on the Fe-N4 sites, which is the origin of the inactivity for the methanol oxidation reaction (MOR). Furthermore, Fe-NLPC was applied to membraneless alkaline direct methanol FC (DMFC) in practice, exhibiting outstanding performance. Meanwhile, the Fe-NLPC-based ZAB also shows excellent electrochemical performance.
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