ADVANCED MATERIALS
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2021
·Vol. 34
·期 5
·2105410
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IF 30.849
Leping Yang,Xu Zhang,Lingxiao Yu,Jianhua Hou,Zhen Zhou,Ruitao Lv
Noble-metal-free, durable, and high-efficiency electrocatalysts for oxygen reduction and evolution reaction (ORR/OER) are vital for rechargeable Zn–air batteries (ZABs). Herein, a flexible and free-standing carbon fiber membrane immobilized with atomically dispersed Fe–N 4 /C catalysts (Fe/SNCFs-NH 3 ) is synthesized and used as air cathode for ZABs. The intertwined fibers with hierarchical nanopores facilitate the gas transportation, electrolyte infiltration and electron transfer. The large specific surface area exposes a high concentration of Fe–N 4 /C sites embedded in the carbon matrix. Modulation of local atomic configurations by sulfur doping in Fe/SNCFs-NH 3 catalyst leads to excellent ORR and enhanced OER activities. The as-synthesized Fe/SNCFs-NH 3 catalyst demonstrates a positive half-wave potential of 0.89 V and a small Tafel slope of 70.82 mV dec –1 , outperforming the commercial Pt/C (0.86 V/94.74 mV dec –1 ) and most reported M–N x /C (M = Fe, Co, Ni) catalysts. Experimental characterizations and theoretical calculations uncover the crucial role of S doping in regulating ORR and OER activities. The liquid-state ZABs with Fe/SNCFs-NH 3 catalyst as air cathode deliver a large peak power density of 255.84 mW cm –2 and long-term cycle durability over 1000 h. Solid-state ZAB shows stable cycling at various flat/bent/flat states, demonstrating great prospects in flexible electronic device applications.
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ACS Sustainable Chemistry & Engineering
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2021
·
IF 8.198
Zhen Zeng,Shang Wang,Jun Cheng,Guangmei Hou,Deping Li,Guifang Han,Lijie Ci
Solid polymer electrolytes (SPEs) are preferable in the pursuit for developing high-energy Li metal batteries due to their inherent flexibility and intimate contact with electrodes. However, continuous interfacial parasitic reactions and undesired Li dendrite growth caused by inhomogeneous plating/stripping of Li+ result in rapid deterioration of an SPE/Li interface. Herein, a novel Zn2+-containing SPE (SPE-xZn) with anionic groups partially tethered on the polymer chains is developed to meet these challenges. During cycling, Zn2+ cations inside the SPE-xZn will gradually migrate to the surface of a Li electrode and then evolve to a Li-Zn alloy layer, where Li+ can diffuse more efficiently. Meanwhile, owing to the electrostatic interaction, the immobilized anionic groups within SPE-xZn can alleviate local concentrated Li+ flux. The synergistic effects of an in situ formed alloy layer and unique macromolecular structure can promote uniform plating/stripping of Li, thus yielding a more stable SPE-xZn/Li interface. Therefore, steady cycling over 300 h at 0.2 mA cm–2 is achieved by Li/SPE-5Zn/Li, and an impressive capacity retention of 87.3% at 0.5 C after 800 cycles is realized by LFP/SPE-5Zn/Li with an average Coulombic efficiency of 99.90%.
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CHEMICAL ENGINEERING JOURNAL
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2021
·
IF 13.273
Haoran Pan,Xinning Huang,Zhenjie Lu,Zhiqiang Zhang,Baigang An,Dongling Wu,Tao Wang,Xingxing Chen,Fangyi Cheng
The development of high-performance non-precious bifunctional electrocatalysts for both the oxygen reduction reaction (ORR) and the oxygen evolution reaction (OER) is urgently needed to realize the commercialization of rechargeable metal-air battery. Herein, we report a ZIF-67 derived hybrid Co-based carbon composite as bifunctional ORR/OER electrocatalyst exhibiting excellent performance and stability in a custom-built Zn-air battery. The catalyst was formed by pyrolytic carbonization of ZIF-67 followed by mild oxidation and sulfurization to a hybrid composite (Co/Co 3 O 4 @CoS-SNC) comprised of multiple active sites including Co-N 4 , Co-N/S-C, C-N/S-C, Co 3 O 4 and CoS, as well as the surface and edge defects in the carbon matrix, that act concertedly yielding a highly efficient bifunctional ORR/OER catalyst for reversible oxygen electrodes. The catalyst affords remarkably low reversible overpotentials and stability not only in a 3-electrode system, but also in a custom-constructed Zn-air battery, exhibiting competitive performance against state-of-the-art bifunctional ORR/OER electrocatalysts reported to date and thus placing it among the best non-precious metal catalysts for reversible oxygen reactions.
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JOURNAL OF POWER SOURCES
·
2020
·
IF 8.247
Dan Wang,Peixia Yang,Hao Xu,Jingyuan Ma,Lei Du,GuoXu Zhang,Ruopeng Li,Zheng Jiang,Yun Li,Jinqiu Zhang,Maozhong An
The Zn-air battery is a promising next-generation battery because of the higher energy density and safety compared with the Li-ion battery. However, the Zn-air battery suffers from huge energy loss and poor cycling performance, which are due to the sluggish kinetics of oxygen reduction/evolution reactions (ORR/OER) and the instability of bifunctional catalysts . The state-of-the-art bifunctional catalyst is the composite of Pt and Ir/Ru oxides, which is hindered by the scarce resource and high cost. Therefore, developing low-cost and high-efficient bifunctional non-noble metal-based catalysts is essential to the deployment of Zn-air batteries. Herein, we report a dual-nitrogen-source mediated pyrolysis route to rationally design and synthesize the hybrid Co/Co–N–C bifunctional catalyst. The tailored catalyst consisting of carbon confined Co nanoparticles and atomically dispersed Co–N–C moiety is identified. Remarkably, the dual-nitrogen-source derived Co/Co–N–C catalyst demonstrates excellent electrochemical performances with a half-wave potential of 0.882 V for ORR and a potential of 1.640 V at 10 mA cm −2 for OER; reasonably, the bifunctionality of Co/Co–N–C, which is supported by the excellent self-breathing Zn-air battery performance (the maximum energy density of 897.1 Wh kg Zn −1 ; no obvious degradation within 167h cycling). The abundant Co-Nx sites and metallic Co nanoparticles synergistically boost the ORR and OER.
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JOURNAL OF POWER SOURCES
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2020
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IF 8.247
Na Xin,Yu Liu,Haoting Niu,Hongye Bai,Weidong Shi
Metal organic frameworks (MOFs) with in situ porous nanostructures and high specific surface area have been widely used in supercapacitors , and the reduced graphene oxide (rGO) nanosheets is an excellent electronic conductor and support in loading other materials. Herein, for the first time, we report the unique Co/Zn-MOF derived Co/Zn–S polyhedron homogeneously embedded between the rGO sheets film as a binder-free electrode for high performance hybrid supercapacitor . Using a mild in situ synthesis method and vulcanization process, a 3D nano-electrode material Co/Zn–S@rGO is prepared by combining Zn 0.76 Co 0.24 S nanoparticles with rGO film. Among them, Co/Zn–S@rGO-7 samples with optimizing ratio deliver a high capacitance of 1640 F g −1 at the current density of 1 A g −1 in 6 M KOH alkaline aqueous electrolyte . The asymmetric supercapacitor (Co/Zn–S@rGO-7//AC) using Co/Zn–S@rGO as the positive electrode and activated carbon as the negative electrode shows an ultra-high energy density of 91.8 W h kg −1 , when the power density is 800 W kg −1 . Moreover, the device also shows a high cycle stability under high current density (90.3% capacity retention after 8000 cycles). It shows that the electrode materials prepared by this method has a good application prospect in electrochemical energy storage .
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Hairus Abdullah,Yu-Rou Ko,Dong-Hau Kuo,Noto Susanto Gultom
La–Sn-codoped Zn(O,S) catalysts were synthesized with different amounts (0%, 2.5%, 5%, and 10%) of Sn and a constant amount (10%) of La to improve the photocatalytic hydrogenation reaction (PHR) of azobenzene to aniline. The as-prepared catalysts were carefully characterized and tested for a hydrogenation reaction. The incorporation of Sn significantly enhanced the PHR activities since the incorporated Sn in the Zn(O,S) lattices could increase the conductivity of the catalysts to improve the charge transfer during the catalytic reaction as indicated with EIS measurement. Further measurement with a photoresponse of La–Sn-codoped Zn(O,S) catalysts also exhibited relatively higher intensities as compared to those of La-doped Zn(O,S) and Sn-doped Zn(O,S) catalysts. On the basis of the measurement results of EIS and transient photo current, the La–Sn-codoped Zn(O,S) with the best properties was further utilized for PHR to convert azobenzene to aniline. GC–MS measurement confirmed that 15 ppm azobenzene could be totally converted to aniline in only 60 min which was achieved with a catalyst that was prepared with 5%-Sn and 10%-La doping. The relatively short reaction time indicated that the as-prepared catalyst had a strong reduction capability able to cleave the strong bonding of N═N in azobenzene. The reaction kinetic of the N═N bond cleavage was elucidated based on solvation, adsorption, pinning, and photocatalytic hydrogenation processes on the catalyst surfaces.
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FUEL
·
2020
·
IF 5.578
Tongxin Qu,Shengli Niu,Xiangyu Zhang,Kuihua Han,Chunmei Lu
The calcium modified Zn-Ce/Al 2 O 3 heterogeneous base catalysts are synthesized by the hydrothermal method, impregnation method and co-precipitation method, respectively. Further, they are applied to catalyze transesterification of palm oil with methanol for the biodiesel production. The hydrothermal method with the Ca: Zn: Ce: Al molar ratio of 5: 4: 1: 1 is preferred to synthesize the catalyst due to the best catalytic performance. The catalyst shows strong reusability, where the biodiesel yield of 87.37% is obtained for the fifth reused cycle and the weakened catalytic capability is mainly ascribed to the leaching out of the active sites. The response surface methodology with the central composite design (RSM-CCD) is employed to optimize the transesterification parameters and predict the biodiesel yield. The predicted maximum biodiesel yield of 99.44% is achieved at the reaction temperature of 66.12 °C, methanol to oil molar ratio of 18.53 and catalyst amount of 8.19 wt. % with 3 h, which is consistent with the experimental result of 99.41%. Also, the physical properties of the produced biodiesel meet the ASTM D 6751 standard. This study reveals the Ca-Ce-Zn/Al 2 O 3 catalyst gains a good application prospect in the biodiesel production and the response surface methodology is effective in optimizing the transesterification parameters and predicting the optimal values.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Yang Liu,Depeng Ji,Mian Li,Jie Xiao,Peng Dong,Chengxu Zhang,Lina Han,Yingjie Zhang
The oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) have a critical function as the cathode reactions in rechargeable Zn-air batteries. In this work, a facile strategy for the scalable fabrication of cobalt nanoparticles encapsulated in nitrogen-doped carbon nanotubes (Co@NC) was used. The experimental results and density functional theory calculations demonstrated that carbon nanotubes with a good graphitization degree were obtained by introducing a certain amount of cobalt species. The Co@NC-3 catalyst exhibited good catalytic performance, with a potential gap (ΔE) between the E j=10 value of the OER and ORR half-wave potential (E 1/2 ) of only 0.816 V, which is lower than that of many highly efficient bifunctional catalysts reported in the literature. Moreover, rechargeable Zn-air batteries based on the Co@NC-3 catalyst generated a high power density (163.4 mW∙cm −2 ) and specific capacity (795.5 mA h∙g −1 at 10 mA∙cm −2 ). The results confirm that Co@NC-3 could be used as a highly efficient bifunctional catalyst for renewable energy conversion devices.
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MICROCHIMICA ACTA
·
2020
·Vol. 187
·期 9
·1-11
·
IF 6.232
Tang Tingting,Yang Fan,Wang Lina,Zhao Chunxin,Nie Fei,GuopingYang
An ultrasensitive sandwich electrochemiluminescence (ECL) biosensor was designed for determination of concanavalin A (ConA) through the specific carbohydrate-ConA interactions. Three-dimensional porous metal-organic framework (Zn-MOF) was synthesized, which loaded a large amount of luminescent reagents as luminol by encapsulating into its pores to form Zn-MOF@luminol complex. Interestingly, Zn-MOF also acted as the coreactant accelerator in the luminol-H 2 O 2 ECL system. This Zn-MOF@luminol complex was used as the signal probe to achieve a super strong and stable ECL signal. In addition, three-dimensional hierarchical molybdenum disulfide nanoflower and multiwalled carbon nanotubes complex (MoS 2 NF@MWCNTs) with peroxidase-mimicking enzyme property were used as a substrate to modify the glassy carbon electrode to further enhance the ECL signal of luminol by promoting decomposition of H 2 O 2 into reactive oxygen species (ROSs). In addition to the horseradish peroxidase (HRP) catalysis effect on the luminol ECL signal, a triple amplified ConA sandwich ECL sensor with high sensitivity sensor was constructed. The linear range for ConA detection was from 0.5 pg/mL to 100 ng/mL with a detection limit of 0.3 pg/mL ( S / N = 3). The recovery test for ConA in human serum samples was performed with satisfactory results.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yingwei Li,Shiwei Weng,Shasha Wang,Guojie Zhang,Fusheng Liu,Mengshuai Liu
The development of novel catalytic materials that integrate multifunctional sites has significant implications for expanding the utilization of CO 2 resources. However, simultaneously achieving high activity and stability remains a formidable challenge. In this study, a series of ZIF-8(Zn/Co)@g-C 3 N 4 nanocomposites were prepared by employing a thermo-physical compounding strategy that involved the combination of nitrogen-rich graphitic carbon nitride (g-C 3 N 4 ) nanosheets with ZIF-8(ZnCo). The influences of different compositions of g-C 3 N 4 and ZIF-8(Zn/Co) on the catalyst structure were systematically investigated. Subsequently, the catalytic activities of these nanocomposites towards the cycloaddition reaction between CO 2 and epoxide were examined under different conditions. The presence of abundant Lewis base sites in g-C 3 N 4 facilitates CO 2 activation, while multiple Lewis acid sites in ZIF-8(Zn/Co) enable efficient epoxide activation. By working synergistically with a co-catalyst, tetrabutylammonium bromide (TBAB), CO 2 and epoxides can be efficiently reacted to synthesize the corresponding cyclic carbonates under mild or even atmospheric pressure conditions. The catalytic reaction conditions were optimized, and both the catalyst's recycling performance and the scope of epoxides with various substituents were investigated. The integration of g-C 3 N 4 and ZIF-8(Zn/Co) endows the catalytic material with exceptional structural stability and remarkable catalytic activity, thereby providing a new platform for highly efficient CO 2 conversion.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Weiwei Wang,Rui Huang,He Peng,Ruiting Hu,Ling Ran,Yu Tao,Li Yani,Jun Yan
The emerging aqueous Zn-ion batteries (ZIBs) with their low price and inherent safety are showing strong competitiveness in the energy storage field. In this work, layer-by-layer stacked amorphous V 2 O 5 @Ti 3 C 2 T x heterostructures anchored on three-dimensional carbon cloth (3D CC), synthesized by annealing process and subsequent in-situ electrochemical induction, are reported as high capacity and stable cathode for ZIBs . In this composite cathode, amorphous V 2 O 5 @Ti 3 C 2 T x synergistic heterostructure provides isotropic Zn 2+ migration channels and rapid electron transfer kinetics, while the 3D CC substrate can ensure that the bulk phase in the electrode material is also utilized to maximize the synergistic effect. As a result, the CC/a-V 2 O 5 @Ti 3 C 2 Ti x cathode achieves a high specific capacity of 567 mAh/g at 0.1 A/g, a satisfactory rate performance of 213 mAh/g at 10 A/g, together with a long cycle life of 96.2 % capacity retention after 2000 cycles. Ex-situ characterizations show that the CC/a-V 2 O 5 @Ti 3 C 2 T x cathode undergoes a highly reversible Zn 2+ /H + co-intercalation/deintercalation mechanism during the discharge/charging process. In addition, based on the CC/a-V 2 O 5 @Ti 3 C 2 T x cathode, the assembled flexible ZIB can operate properly under different bending degrees, showing its practicality in flexible devices. This work provides insight into the rational design of cathode materials with high Zn-storage performance.
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Surfaces and Interfaces
·
2023
·
IF 6.2
A.V. Ravindra,M. Chandrika,Andem Sandeep
This work presents the effectual degradation of MB and MO dyes in an aqueous solution under UV light irradiation on nano ZnFe 2 O 4 , NiFe 2 O 4 , and Fe 3 O 4 without using any supplementary oxidants has been reported. Nano ZnFe 2 O 4 , NiFe 2 O 4 , and Fe 3 O 4 are successfully prepared via a co-precipitation technique utilizing biodegradable starch as a surfactant . XRD patterns reveal a pure spinel phase for all the samples. FTIR spectra confirm the successful embedding of the starch surfactant. SEM micrographs exhibit tiny spherical particles of size 5–8 and 4–6 nm for ZnFe 2 O 4 and NiFe 2 O 4 but spherical particles of 8–10 nm and flake-like particles of ∼14 nm thick for Fe 3 O 4 . N 2 sorption studies show type-IV isotherms typical of mesoporous structures. The direct bandgap of these ferrite nanoparticles is 2.03–2.15 eV, related to the metal D-d onsite transfers, which are permitted by spin but prohibited by parity. MB decolorization of 99% is achieved in less than 2 h for all the samples; in contrast, MO decolorization takes relatively longer irradiation. The decolorization kinetics suggests that the pseudo-second-order model is more appropriate to explain the decolorization process of MB and MO by the catalysts. The order of photocatalytic activity evaluated from rate constant (k 1 ) per SSA values is Fe 3 O 4 < ZnFe 2 O 4 < NiFe 2 O 4 for both MB and MO decolorization. NiFe 2 O 4 photocatalyst shows the best effect on the decolorization of both dyes due to its low bandgap and high surface area. All the ferrite catalysts demonstrate high stability with no substantial deterioration of photocatalytic activity even after three cycles. The results of this study endorse that the nano ferrites prepared in this work are potential candidates for the photocatalytic degradation of aqueous solutions of MB and MO.
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