Nano-Micro Letters
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2022
·Vol. 14
·期 1
·1-13
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IF 23.655
Shang Wenshuo,Li Qiang,Jiang Fuyi,Huang Bingkun,Song Jisheng,Yun Shan,Liu Xuan,Kimura Hideo,Liu Jianjun,Kang Litao
Highlights
High-performance Zn||I 2 batteries were established by coating zeolite protecting layers.
The Zn 2+ -conductive layer suppresses I 3 − shuttling, Zn corrosion/dendrite growth.
The Zeolite-Zn||I 2 batteries achieve long lifespan (91.92% capacity retention after 5600 cycles), high coulombic efficiencies (99.76% in average) and large capacity (203–196 mAh g −1 at 0.2 A g −1 ) simultaneously.
Abstract The intrinsically safe Zn||I 2 battery, one of the leading candidates aiming to replace traditional Pb-acid batteries, is still seriously suffering from short shelf and cycling lifespan, due to the uncontrolled I 3 − -shuttling and dynamic parasitic reactions on Zn anodes. Considering the fact that almost all these detrimental processes terminate on the surfaces of Zn anodes, modifying Zn anodes’ surface with protecting layers should be one of the most straightforward and thorough approaches to restrain these processes. Herein, a facile zeolite-based cation-exchange protecting layer is designed to comprehensively suppress the unfavored parasitic reactions on the Zn anodes. The negatively-charged cavities in the zeolite lattice provide highly accessible migration channels for Zn 2+ , while blocking anions and electrolyte from passing through. This low-cost cation-exchange protecting layer can simultaneously suppress self-discharge, anode corrosion/passivation, and Zn dendrite growth, awarding the Zn||I 2 batteries with ultra-long cycle life (91.92% capacity retention after 5600 cycles at 2 A g −1 ), high coulombic efficiencies (99.76% in average) and large capacity (203–196 mAh g −1 at 0.2 A g −1 ). This work provides a highly affordable approach for the construction of high-performance Zn-I 2 aqueous batteries.
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DALTON TRANSACTIONS
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2022
·Vol. 51
·期 14
·5624-5634
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IF 4.569
Jia Wang,Xiange Huang,Hegen Li,Deyue Yan,Wei Huang
Here two Zn(II) coordination polymers [Zn20(DMCA)12]O12 (DMCA = demethylcantharic acid, DMCA-Zn1) and [Zn(DMCA)](H2O)2 (DMCA-Zn2) are synthesized from a broad-spectrum anticancer drug norcantharidin (NCTD) and Zn(NO3)2·6H2O under solvothermal conditions. By mechanical grinding with a biocompatible polymeric surfactant F127, ultrasonic treatment and filtration, DMCA-Zn1 and DMCA-Zn2 can be transformed into stable nanoparticles (DMCA-Zn1 NPs and DMCA-Zn2 NPs) suspended in water with average diameters of around 190 nm and 162 nm for drug delivery. The in vitro evaluation indicates that DMCA-Zn1 NPs and DMCA-Zn2 NPs can enter into HepG2 and Hep3B cancer cells via endocytosis and inhibit their proliferation. Meanwhile they exhibit relatively low toxicity to L927 normal cells. The in vivo evaluation confirms that DMCA-Zn1 NPs and DMCA-Zn2 NPs can more effectively inhibit the growth of Hep3B tumors with relatively few side effects compared with free NCTD. This approach can be extended to other anticancer drugs to construct nanodrug delivery systems for cancer treatment.
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Materials Today Energy
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2022
·
IF 9.257
Xinxin Bian,Bowen Liu,Xiaolei Wang,Zhimin Chen,Rui Gong,Wanqi Jia,Zichen Song,Huiyuan Meng,Weibo Yin,Zhiyu Ren
Defects engineering is one of the effective strategies to advance the CO 2 conversion into value-added chemicals and fuels during the electrochemical process. It is noteworthy that multiple defects are often associated in the reaction process, hence how to stimulate their synergistic effect is extremely important, but still lacks in-depth understanding. Herein, SnO 2 nanosheets with simultaneous oxygen vacancies and Zn dopants (Zn–Vo–SnO 2 ), as a proof-of-concept study, were proposed to elucidate the synergistic effect of multiple defects on enhanced CO 2 -to-C 1 conversion. Zn–Vo–SnO 2 , which is prepared by coupling a facile hydrothermal reaction and a subsequent desulfurization, yields the C 1 products at the lower applied potential, and maintains the FE C1 of about 95% at −0.80 V vs. RHE for a long-term operation. Evidences from systematic experiment and theoretical calculation corroborate that the charge redistribution caused by the oxygen vacancies and Zn-doping synergistically energize the CO 2 conversion, in the term of the CO 2 adsorption, the hydrogenation of CO 2 and intermediates, and the thermodynamic energies of the rate-determining steps. This study has an insight into defect engineering to design advanced electrocatalysts for implementable CO 2 recycling and utilization.
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OPTICAL MATERIALS
·
2022
·
IF 3.754
Si Wu,Huicong Liang,Zhe Zhang,Qi Zhang,Qiang Han,Jingshu Wang,Ming Gao,Hougang Fan,Jinghai Yang,Jihui Lang
Zn–Al layered double hydroxides (Zn–Al LDHs) with a typical layered structure were successfully synthesized by the hydrothermal method . The effects of molar ratios of Zn and Al on the structure, morphology, chemical composition and photocatalytic performance of Zn–Al LDHs were systematically investigated. By adjusting the Zn/Al molar ratio, it can be found that the Zn–Al-LDH-3 sheet with the ratio of 3 exhibits the best photocatalytic activity and reusability, which is mainly ascribed to the formation of more photo-generated holes in the photocatalytic process proved by the free radical quenching experiment. The optimized conditions of catalyst dosages, rhodamine B (RhB) concentrations and initial pH values to achieve the highest were also investigated in detail. This work provides a simple method for designing environmental friendly layered double hydroxide photocatalysts with special morphologies.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Bareera Raza,Yang Zhang,Ming Xu,Jun Yang,Yanna NuLi,Jiulin Wang
Rechargeable Zinc batteries as energy storage and conversion devices are attracting wide attention due to their merits of intrinsic safety, abundant resources, and inexpensive components. However, the thermodynamic instability of Zn metal anode in the aqueous environment leads to limited cycle life, poor rechargeability, and restricted large-scale employment of Zinc batteries. Herein, we investigate the electrochemical and morphological behavior of Zn anode in an organic aprotic amide, N’N -dimethylacetamide (DMAC) solvent-based electrolyte, which demonstrates highly reversible Zn deposition (CE of ∼ 99.80%), improved anodic stability (∼2.4 V vs. Zn/Zn 2+ ), and a high current capability of 15.0 mA cm −2 /15.0 mAh cm −2 . Practically, a remarkable performance with high-capacity retention and high CE (≥99%) is attained for Zn||MnO 2 full cell, which is a positive step toward the development of rechargeable Zinc batteries.
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Sustainable Chemistry and Pharmacy
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2022
·
IF 5.464
Zhenwei Zhang,Xiaoshi Ma,Chuanjun Yue,Xuejiao Wei,Baoliang Liu,Xiaohui Chen
Hazardous waste alkaline batteries and waste fatty acids significantly threaten the environment. In this study, waste alkaline batteries were simply transferred to r-MnZn catalysts, which were then applied in the ketonization of fatty acids. The assessment results show that r-MnZn can efficiently convert n-octanoic acid to 8-pentadecanone. The conversion and yield are evaluated as 100% and 92.9%, respectively, which are much better than those of TiO 2 , ZrO 2 , CeO 2 and other metal oxides . The excellent catalytic efficiency is derived from the MnO 2 nanorods in r-MnZn materials which are characterized by XRD, TEM, and XPS. In addition, when using different kinds of fatty acids in ketonization, longer carbon chains require a higher activation energy, and the conversion of fatty acids was lower. Furthermore, the ketone products have a short carbon chain that induces side reactions, leading to a low yield. The above results indicate that r-MnZn is an efficient catalyst applied in the ketonization of fatty acids.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Chen Li,Yue Jia,Xiaolong Lu,Huayan Chen
Recovery of heavy metal ions from waste water has benefits both in terms of resources reuse and environmental protection. Polymer inclusion membrane (PIM) has received increasing attention as a gentle and simple method compared to other separation techniques for the removal and recovery of heavy metal ions. The extractant and matrix are the most important components of the PIM. In this paper, a novel matrix enhanced polymer inclusion membrane (ME-PIM) system containing both octyl hydroxamic acid (OHA) and di (2-ethylhexyl) phosphoric acid (D2EHPA) as the carriers as well as poly(vinyl) chloride (PVC) and poly (vinylidene fluoride- co -chlorotrifluoroethylene) (PVDF-CTFE) as the matrix was reported. The SEM results indicate that the PVC has excellent compatibility with OHA and D2EHPA, resulting in dense ME-PIM compared to PVDF-CTFE. The effects of OHA and D2EHPA with different carrier ratios on the transport and the stability of the membrane were examined using Zn (Ⅱ) as a representative of heavy metal ions. The optimal results of this work showed that the initial mass transfer flux value of Zn (Ⅱ) was as high as 4.73 μmol/(m 2 ·s), corresponding to a permeability of 2.21 × 10 −2 m/h, using the ME-PIM composed of 61 wt.% PVC and 22 wt.% OHA + 17 wt.% D2EHPA. All these results suggest that the ME-PIM has a much higher initial mass transfer flux than those of PIMs in literatures. The addition of OHA to PIM introduced extractive functional groups into the polymer chain, forming an efficient and progressive mass transfer path with the extractant D2EHPA. Utilizing two extractants with synergistic effects, this novel ME-PIM system provides a potential advantage in promoting the mass transfer of metal ions in a PIM.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
·
IF 4.539
Kun Jiang,Kun Liu,Qian Peng,Muyang Zhou
Montmorillonite (MMT) and humus have a good adsorption effect on heavy metal ions . This study proposed a synthetic method for a novel composite of humus-like substances/MMT (HLS-MMT) by introducing humus precursors into the interlayer domain of MMT and then forming HLS through in situ catalytic polycondensation reaction. The structure and morphology of samples were characterized by XRD , FTIR, and SEM , which demonstrated the successful loading of HLS on the internal and external surfaces of MMT. The experimental results showed that the loading of HLS on MMT was very stable, and the adsorption capacity of the modified MMT for lead and zinc ions was greatly enhanced. The effects of single-factor experiments showed that the pH value was the key factor affecting the adsorption process . In addition, the adsorption process was found to be in good agreement with the Langmuir isotherm model and the pseudo-second-order kinetic model . The competitive adsorption experiment displayed that HLS-MMT had a higher affinity for Pb ions than Zn ions, and the cycling experiment presented that the adsorbent had good regeneration and cycling performance. This study shows that HLS-MMT is a novel adsorbent with a good capacity to separate and enrich Pb and Zn ions similar to ion-exchange resin.
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FUEL
·
2021
·
IF 6.609
Chengming Huang,Dingmei Han,Linjie Guan,Linhua Zhu,Yi Mei,Dedong He,Yun Zu
Propane dehydrogenation (PDH) is a prospective benign process for the production of propylene, but generally depends on high-price Pt and toxic Cr(VI) catalysts that often suffer from the rapid deactivation derived from metal sintering and severe coke deposition. To overcome these problems, the breakthroughs in an alternative catalyst design with efficient, low-cost and eco-friendly play a crucial role in successfully developing this process. Here, we facilely fabricate the bimetallic-site catalyst of Ni-Zn anchored in the zeolitic framework of silicalite-1 (depicted as NiZn-S-1) by employing ligand-protected strategy, which performs high temperature stability. Under comparable conditions, the NiZn-S-1 catalyst with high Ni/Zn molar ratio of 3:1 (named 0.2Ni0.06Zn-S-1) exhibits superior catalytic activity (initial propane conversion of 32.5 % and actual TOF propane of 28.5 min −1 ) with low deactivation rate (0.0778 h −1 ) and great propylene selectivity (>90%) after 30 h on stream. In particular, the catalytic performance on this catalyst almost keeps same as that of fresh catalyst after 4 successive oxidation–reduction cycles. Multiple characterizations further demonstrate that the enhancement of PDH performance ought to be attributed to the synergistic effect between bimetallic Ni-Zn sites, which favors the selective activation of C–H bond and propylene desorption to reduce the formation of coke species with high graphitization degree, boosting the improvement of catalyst stability. The design of novel bimetallic-sites catalyst can give a new idea on the development of alternative PDH catalysts with economical- and environment-friendly in the future.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Huizhen Lv,Yu Song,Zengming Qin,Mingyue Zhang,Duo Yang,Qing Pan,Zhihui Wang,Xinjian Mu,Jianming Meng,Xiaoqi Sun,Xiao-Xia Liu
The disproportionation of the Jahn-Teller (J-T) active manganese oxides (Mn 3+ ) often leads to uncontrollable Mn 2+ dissolution, which has been identified as one of the major causes of the performance degradation in conventional Zn-MnO 2 batteries. Herein, we use the “unwanted” disproportionation of the Mn 3+ cations to realize effective MnO 2 /Mn 2+ transformation, achieving high specific capacity (550 mAh g −1 ) and good cycling stability (5000 cycles without capacity decay) in a Zn-MnO 2 hybrid battery with mild aqueous electrolytes. Mechanism study shows that MnO 2 is deposited on the cathode during charging, H + /Zn 2+ insertion and disproportionation occur sequentially during discharging, leading to Mn 2+ dissolution. The generated high-valence manganese oxides via disproportionation further experience reduction-disproportionation-dissolution, which proceeds repeatedly in the expanded discharge potential to 0 V vs. Zn 2+ /Zn, resulting in the complete dissolution of the cathodic materials. Our results provide the fundamental understanding on the controversial mechanisms of Zn-MnO 2 batteries with mild aqueous electrolytes and highlight the effect of disproportionation in pushing the electrochemical performance of the promising Zn-MnO 2 hybrid batteries.
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SOLID STATE IONICS
·
2021
·
IF 3.785
Fengjiao Guo,Song Gao,Chenchen Ji,Hongyu Mi,Han Li,Wentao Zhang,Huan Pang
Flexible aqueous Zn-ion batteries have aroused great interest as an emerging energy storage technology in smart/wearable electronics due to their low cost, high energy density , good safety, and flexibility. However, the construction of excellent cathode and anode is still a key step for the Zn-ion batteries development. Herein, we report a rechargeable flexible quasi-solid-state (FQSS) Zn-ion battery assembled with free-binder polyaniline/molecular-decorated carbon cloth (PANI/mCC) cathode and zinc nanosheet/CC (Zn/CC) anode sandwiched by poly(vinyl alcohol)/Zn(CF 3 SO 3 ) 2 gel electrolyte. The nanostructured PANI arrays and Zn sheets oriented on the flexible substrates afford rapid transport channels for electrolyte ions and endow electrodes enough flexibility. Consequently, the constructed FQSS Zn-ion battery exhibits outstanding energy/power densities of 185.7 Wh kg −1 /9742 W kg −1 and good capacity retention of 80% after 1000 charge-discharge cycles at 3.3 C. Impressively, the assembled flexible device can accommodate a series of bending states and show stable performance.
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INORGANIC CHEMISTRY
·
2021
·
IF 5.165
Hao-Jing Ding,Ying Zhang,Xi Wang,Qiu-Ying Lin,Shu-Ming Zhang,Mei-Hui Yu,Ze Chang,Xian-He Bu
The construction and modulation of hierarchical pore structure in metal-organic frameworks (MOFs) has become a hot topic owing to the advantages of hierarchical pore MOFs (HP-MOFs) in matter storage and mass transfer related applications. Herein, we report the engineering of crystalline defect in a bimetallic MOF for the construction and tuning of HP-MOF. A microporous MOF system showing metal-center-dependent water stability, namely, {[M3F(bdc)3 tpt] (solvents)}n (M = Zn2+ and Ni2+, H2bdc = 1,4-benzenedicarboxylic acid, tpt = 2,4,6-tris(4-pyridyl)triazine), was utilized as a platform for the construction of HP-MOF. By tuning the Zn2+/Ni2+ ratio in the reactant, a bimetallic MOF with a highly tunable Zn2+/Ni2+ ratio could be obtained. The relatively labile Zn2+-based coordination bonding in the bimetallic MOF could be readily and targeted broken through water treatment for the engineering of crystalline defects-based hierarchical pore structure. The resultant HP-MOF reveals a dramatically increased pore volume with the presence of mesopore and macropore. In addition, the anionic framework of HP-MOF could be utilized for the selective adsorption of a cationic dye methylene blue, and a relatively high capacity (250 mg·g–1, five times compared with the pristine microporous MOF) could be achieved.
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