ACS Nano
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2022
·
IF 18.027
Huaming Yu,Yuejiao Chen,Weifeng Wei,Xiaobo Ji,Libao Chen
Aqueous Zn metal batteries suffer from rapid cycling deterioration due to the severe water corrosion and dendrite growth on Zn anodes. Herein, a highly antiwater Znx-diethylenetriaminepenta(methylene-phosphonic acid) interface layer with good zinc affinity and special nanoscaled 3D granular structure is designed on Zn metal to address these problems. Experimental results combined with theoretical analysis and COMSOL simulations reveal that the hydrophobic groups in such Zn-based organic complex are the decisive factor in preventing H2O from damaging Zn anode surface. The massive Zn2+ attractive sites formed by interaction of methylene-phosphonic acid groups and Zn cause ion channel for fast zinc-ion adsorption and migration. And the developed nano granular architecture on the surface induces redistributed Zn2+ ion flux to realize homogenization with smooth and compact surface deposition. Under the synergism, such modified anodes exhibit long cycling lifespan over 1300 h with a relatively low polarization voltage at 5 mA cm–2. Also, the assembled full cells (including Zn//V2O5 and Zn//MnO2 cell) based on this anode are also demonstrated. The work provides a simple, low cost, and efficient pathway by combining the two concepts of structural design and constructing protective layers on the surface to prepare high-performance Zn anodes toward prospering aqueous zinc–metal batteries.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yan Zhang,Shangyong Zhou,Xing Liu,Peixin Zhang,Zhihong Yan,Jianguo Hu,Ziqi Wei,Lihua Chen,Jun Wang,Shuguang Deng
Efficient separation of ethane (C 2 H 6 ) from ethylene (C 2 H 4 ) using C 2 H 6 -selective adsorbents is more efficient but challenging due to their similar physical and chemical properties. Herein, we report a Zn (II) cluster-based metal-organic framework, Zn 4 O(NTB) 2 , with suitable cavity pockets and favorable adsorption sites for the reverse capture of C 2 H 6 from C 2 H 6 /C 2 H 4 mixtures. Both high C 2 H 6 uptake (2.83 mmol g −1 ) and C 2 H 6 /C 2 H 4 selectivity (2.06) at 273 K and 1 bar was achieved, outperforming many top-ranking C 2 H 6 -selective adsorbents. Moreover, dispersion-corrected density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulation revealed that C H···O and C H···π interactions are formed with C 2 H 6 in the suitable pockets with saturated Zn clusters and nonpolar pore surfaces. Dynamic breakthrough experiments demonstrated its practical separation performances with various gas-mixture compositions and those containing water vapor.
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TALANTA
·
2022
·
IF 6.556
Mingxing Liu,Rongrong Jiang,Meie Zheng,Mengjiao Li,Qingjie Yu,Hongda Zhu,Huiling Guo,Hongmei Sun
A sensitive unlabeled ratiometric biosensor was developed to the detection of cardiac troponin I (cTnI). This biosensor was established by using the glassy carbon electrode coated with graphene oxide to form a platform bonded with N, Zn co-doped graphene quantum dots (N, Zn-GQDs). The N, Zn-GQDs was successfully prepared as the raw materials of graphite powder and characterized. Antibodies of cTnI were bonded to the surface of N, Zn-GQDs as the nanoprobe by amide bonds. The signals of electrochemiluminescence (ECL) and differential pulse voltammetry (DPV) were exposed to decrease in the presence of cTnI, which caused the signal substance to move farther away from the electrode. It was found that the immune complex layer attenuated the intensity of ECL and DPV which could be used as the good overall signal for determining concentration of cTnI. The ratiometric biosensor had a good response to cTnI with the detection limit is 4.59 pg L −1 in the concentration range of 10–10 6 pg L −1 . The developed method was evaluated for the detection of cTnI in human serum, and the obtained results were consistent compared to the reference values obtained by hospital standard enzyme linked immunoassay (ELISA) with 9.09%–11.1% of RSD. Our findings suggested that this ratiometric biosensor could be used to the detection of cTnI in human serum with lower cost and higher sensitivity, it also might be better potential application prospect based on N, Zn-GQDs to detect other biomarkers.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Yu Wang,Feng Gu,Lei Cao,Lanlan Fan,Tianjie Hou,Qian Zhu,Yu Wu,Shixian Xiong
Developing non-noble metal oxygen reduction reaction (ORR) electrocatalysts with high performance, excellent stability, and low-cost is crucial for the industrialization of fuel cells. Herein, trace level Co modified 3D hybrid titanium carbonitride MXene and boron-carbon-nitrogen nanotubes catalyst (TiCN–BCN–Co) is fabricated by spray-lyophilization and high-temperature pyrolysis . This strategy not only avoids the oxidation of Ti 3 C 2 T x MXene, but also introduces nitrogen atoms into the titanium carbide lattice to form a more electrocatalytically active TiCN crystal phase. The obtained TiCN–BCN–Co exhibits superior ORR catalytic activity with a positive half-wave potential of 0.83 V vs. RHE and outperforms commercial Pt/C in terms of stability and methanol tolerance. Impressively, the Zn-air battery with TiCN–BCN–Co cathode achieves a superior specific capacity of 791 mAh g −1 and long-term stability of 200 h.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Mei-Mei Wang,Li-Juan Liu,Jia-Rui Xi,Ying Ding,Peng-Xi Liu,Liang Mao,Bing-Jie Ni,Wei-Kang Wang,Juan Xu
The presence of oxygen vacancies (OVs) promotes persulfate activation. However, rational modulation of OVs without compromising the inherent structure of catalysts is challenging. Herein, novel OVs-enriched hollow ZnCo 2 O 4 nanocages are synthesized based on a bimetallic ZIF-67@ZIF-8 precursor for efficient peroxydisulfate (PDS) activation. The incorporation of Zn into the lattice of Co 3 O 4 boosts the number of OVs in the catalysts while preserving the morphology of Co 3 O 4 nanocages derived from metal-organic framework (MOFs) templates. As a result, the degradation rate of organic pollutants such as bisphenol A is improved by over 20 times in the developed PDS activation system. OVs promote the formation of a surface-activated complex from PDS onto the catalyst surface, which can subsequently deprive electrons from pollutants. The developed PDS activation system is resistant to Cl − , NO 3 − and humic acid at environmental concentrations. This system adapts to selectively degrade organic pollutants with low ionic potential, and shows applicable potential in practical packaging wastewater treatment. The decreased catalytic performance of catalysts during utilization can be recovered with a facile thermal treatment. Our work constructs OV active sites on Co 3 O 4 nanocages while preserving their original structural superiorities, providing a new strategy to functionalize MOF-derived materials.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Shaotang Dong,Guoqing Xiao,Chunlin Chen,Chunyan Chen,Zhengwei Yang,Fei Zhong,Mingtan Wang,Rui Zou
Layered double hydroxides acts as an effective inorganic nano-fire retardant, which is capable of releasing water, carbon dioxide and diluting the concentration of combustible gases when encountering flames, thus providing fire protection. Here, zinc-aluminum layered double hydroxides (Zn-Al/LDH) is uniformly anchored on the reduced graphene oxide (RGO) surface by a simple hydrothermal strategy in order to further enhance the barrier effect of the char layer. The obtained Zn-Al/LDH anchored reduced graphene oxide (Zn-Al/LDH@RGO) hybrids were added to waterborne epoxy resin and their fire resistance properties were measured by large plate combustion test, furnace storage test and thermal weight loss test. The results showed that the incorporation of nano-fillers effectively enhanced the fire resistance of the composite coatings . Among them, Zn-Al/LDH@RGO -based fireproof coatings presented better fire performance due to the active flame retardant mechanism of Zn-Al/LDH and the high barrier property of RGO nanosheets . In contrast, the composite coating with 1.5% of Zn-Al/LDH@RGO hybrids had the lowest backside temperature of 154.3 °C. Besides, the Zn-Al/LDH@RGO/EP (1.5%) coating also exhibited the highest expansion height (16.5 mm), expansion rate (12.13) and the highest char residue rate (32.2%), indicating its highest fire retardant performance.
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LUMINESCENCE
·
2021
·Vol. 37
·期 1
·72-81
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IF 2.464
Haonan Zhao,Junfeng Zhang,Xiaolian Lin,Huihui Li,Qinhe Pan
Cr(VI) is a type of dangerous effluent that has caused great harm to human health and the environment. Recognition and perception of Cr(VI) by artificial receptors has attracted extensive attention. A novel fluorescent chemical sensor based on the 5,7-dihydroxyflavone skeleton was designed and synthesized for the selective recognition of Cr(VI). As confirmed by fluorescence technology, the fluorescent probe 4-dimethylaminobenzyl chrysin ester–Zn (DBC–Zn) showed high sensitivity and selectivity for dichromate and a fast response (less than 30 sec) recognition. The fluorescence intensity of DBC–Zn varies linearly with the concentration of Cr(VI) in the range 0.1–1 μM. The detection limit of Cr 2 O 7 2− by DBC–Zn is 2.3 nM, which is far lower than the national safe drinking water standard stipulated by the US Environmental Protection Agency (1.9 μM). The quenching mechanism of the probe can be attributed to the interaction of the dynamic quenching effect and the fluorescence internal filtration effect. In addition, the probe has good stability in both neutral and alkaline environments, and the accuracy of quantitative analysis of Cr 2 O 7 2− in lake water or tap water is more than 80%. The test paper based on DBC–Zn can effectively detect Cr 2 O 7 2− at the concentration of 100 ppb. This shows that the probe has a certain practical application value.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Siyuan Zhao,Tong Liu,Yawen Dai,Yang Wang,Zengjia Guo,Shuo Zhai,Jie Yu,Chunyi Zhi,Meng Ni
The low operating voltage of 1.4 V limits the widespread application of flexible Zn-air batteries (ZABs) in wearable electronics. However, a high-voltage flexible ZAB has not been achieved yet, which results from the few choices of fitted flexible electrolytes. Now we propose a novel, universal, and simple strategy to design all-in-one and membrane-free acid-alkaline flexible electrolytes based on thermo-reversible Pluronic® F127 hydrogels. Benefiting from the unique sol–gel transition property of Pluronic® F127 hydrogel, the acid and alkaline can be decoupled but integrated simultaneously in one hydrogel. Surprisingly, the as-developed ZAB achieves an unprecedentedly high voltage of 2 V, surpassing all the existing flexible ZABs. Meanwhile, this battery exhibits remarkable high-voltage stability of 37 h and a large area capacity of 1.35 mAh cm −2 without the use of costly bipolar membranes. Our work presents a pioneering example for flexible high-voltage ZAB and may further inspire other designs of flexible high-voltage aqueous batteries and decoupled dual-electrolyte batteries.
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CHEMICAL ENGINEERING SCIENCE
·
2021
·
IF 4.311
Juan Cui,Yiming Leng,Zhonghua Xiang
Developing low-cost and excellent performance bifunctional catalysts for Oxygen Reduction Reaction (ORR) and Oxygen Evolution Reaction (OER) in rechargeable Zn-air batteries is of great significance. Recently, metal organic frameworks (MOFs)-derived electrocatalysts have been widely studied in ORR and OER due to their large specific surface area and tunable pore structure. However, it is still a challenge to prepare hierarchical porous structure catalysts via facile approach, which is desired in the device manner. Herein, we synthesized a MOF-derived FeNi co-doped catalyst (termed as B-FeNi-N/C-1000) using the binary ligand strategy with a large specific area and suitable hierarchical pore structures which efficiently improves mass transfer to boost the high device performance. As a result, the B-FeNi-N/C-1000 exhibits an outstanding ORR performance with a half potential of 0.9 V vs. RHE and a low potential of 1.62 V vs. RHE at 10 mA cm −2 in alkaline media, which exceeds FeNi catalyst (i.e., FeNi-N/C-1000) via single ligand method and commercial Pt/C + IrO 2 . Additionally, the B-FeNi-N/C-1000 presents a higher power density of 102 mW cm −2 and a long-term stability that only losses 2% after 95 h in the self-assembly Zn-air battery. Accordingly, this work can provide a facile method to synthesize efficient bifunctional catalyst for, but not limit to Zn-air flow batteries.
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Materials Today Energy
·
2021
·
IF 7.311
Fangfang Wu,Youwei Wang,Pengchao Ruan,Xinxin Niu,Dong Zheng,Xilian Xu,Xiaobin Gao,Yanhui Cai,Wenxian Liu,Wenhui Shi,Xiehong Cao
Vanadium-based oxides with high theoretical specific capacity and open crystal structure are promising cathodes for aqueous zinc ion batteries . However, the frustrating dissolution and structural collapse of vanadium-based oxides, especially when cycling at a low current density, lead to severe performance degradation. Here, we demonstrate doping of Fe opens up a rapid Zn 2+ diffusion channel, and results in a stable layer-structured vanadium oxide nanobelt (FeVO) with an expanded interlayer spacing up to 10.8 Å. This enables a cathode with high structural stability, leading to an outstanding cyclic stability of 300 cycles at a low current density of 0.5 A g −1 with a high retention of 94.6%. Even cycling at 0.2 A g −1 , the Fe-doped vanadium oxide still maintains a retention of 93.6% after 150 cycles. A reversible co-intercalation mechanism of Zn 2+ and H 2 O is further revealed via ex - situ X-ray powder diffraction (XRD) and X-ray photoelectron spectra techniques. Such boosted electrochemical performance is attributed to the large interlayer space providing ion diffusion path and a stable layered structure. These excellent characteristics of the prepared vanadium oxide cathode show great potential for high-performance aqueous zinc ion batteries.
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Nature Communications
·
2021
·Vol. 12
·期 1
·1-12
·
IF 14.919
Xie Chao,Lin Longfei,Huang Liang,Wang Zixin,Jiang Zhiwei,Zhang Zehui,Han Buxing
Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn 2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn 2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.
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FUEL
·
2021
·
IF 6.609
Tao Pan,Sida Ge,Mengnan Yu,Yana Ju,Ran Zhang,Pei Wu,Kuanyu Zhou,Zhijie Wu
Zn modified ZSM-5 zeolite supported Ni bifunctional catalysts were prepared by in-situ hydrothermal synthesis (Zn-Ni-ZSM-5), co-impregnation method (Zn-Ni/ZSM-5) as well as combining in-situ hydrothermal synthesis of Zn-ZSM-5 and sequential impregnation of Ni (Ni/Zn-ZSM-5) and used for the selective converting olefin to aromatics applicable for FCC gasoline hydro-upgrading. The Lewis (L) acid sites generated by ZnOH + species and hydrogenation active sites from Ni 0 species were varied with preparation method, in which their locations at the external surface or micropores of zeolite changed the acid properties of catalysts. Comparing to the Zn-Ni/ZSM-5 from the co-impregnation method, direct in-situ hydrothermal method could incorporate Zn and Ni species within zeolite, which makes the strong interaction between the metal species and the framework Al to form medium-strong L acids (ZnOH + /NiOH + ). This leads to the decrease of ratio of Brønsted acid sites to L acid sites (B/L) from 0.40 to 0.12 and the difficulty in reducing of Ni cations to Ni 0 from 57% to 30% Ni 0 percent. Ni/Zn-ZSM-5 sample prepared by incorporating Zn species into micropores and sequential depositing Ni species at the external surface of zeolite possesses a low B/L ratio similar to Zn-Ni-ZSM-5 (0.20 versus 0.12) but a much higher Ni 0 percent (52% versus 30%). Zn-Ni-ZSM-5 shows closer intimacy between Zn and Ni species comparing to Zn-Ni/ZSM-5 and Ni/Zn-ZSM-5. For the 1-hexene aromatization, the formed iso -alkene at acid sites was quickly saturated to iso -alkanes by the adjacent Ni 0 particles over Ni-Zn-ZSM-5 catalyst in hydrogen steam. However, the location of aromatization active sites (ZnOH + , L acid sites) in micropores and hydrogenation active sites (Ni 0 species) on external surface of Ni/Zn-ZSM-5 makes the tandem conversion of n-alkene → iso -alkene → aromatics, rather than the n-alkene → iso -alkene → iso -alkane. Thus, Zn-Ni-ZSM-5 with close intimacy of ZnOH + and Ni 0 particles shows a high iso -alkane selectivity (27.9% iC 4 + ), while Ni/Zn-ZSM-5 exhibits a high aromatics selectivity (39.6 %) in the conversion of 1-hexene in hydrogen steam. Similar results have also found in the conversion of n-heptane. Here, the control of the intimacy of Zn and Ni in ZSM-5 zeolites has been realized to be a good protocol to adjust the selective conversion of olefins/alkanes to aromatics versus iso -alkanes.
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