ADVANCED FUNCTIONAL MATERIALS
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2024
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IF 18.5
Jianqiang Weng,Wenqi Zhu,Kun Yu,Jing Luo,Meixin Chen,Liuyan Li,Yuhang Zhuang,Kailai Xia,Zhixing Lu,Yajie Hu,Chengkai Yang,Mingmao Wu,Zhigang Zou
Owing to zinc dendrites and parasitic reactions, aqueous Zn-metal batteries often suffer from poor reversibility and cyclability. Electrolyte additives present a promising strategy to improve Zn anode stability. However, the ever-evolving perspectives and mechanisms, paradoxically, complicate battery design, causing a scenario where any electrolyte additive seems to be effective. Herein, it is taken ionic liquid (IL) additives as an example and detailed explored the impact of three typical IL anions, namely OTF − , TFA − , and BF 4 − . It is identified that the primary determinant of electrolyte additives as their electrical double layer (EDL) structures and their subsequent solid-electrolyte interface (SEI) composition. An advantageous EDL structure, akin to an ion-shield, can reduce the absorption of H 2 O molecules, which further enrich the SEI with zincophilic and hydrophobic components, thereby mitigating parasitic reactions and Zn dendrite formation. As a result, the Zn||Zn cell with optimal [EMIM]OTF additives demonstrates an exceptional cycling life under challenging conditions, its cumulative plated capacity surpasses most previously reported results by utilizing different IL additives. This work extends beyond performance enhancements, representing a valuable exploration of key criteria for electrolyte additives is believed. These insights are expected to offer fundamental guidance for future research and electrolyte design.
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JOURNAL OF POWER SOURCES
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2024
·
IF 8.1
Xiaojie Tan,Fengliang Cao,Xuan Han,Libo Wang,Zhengqiu He,Jinqiang Zhang,Yikun Zhao,Wei Deng,Hui Ning,Zhongtao Li,Qingshan Zhao,Mingbo Wu
Iron-nitrogen-carbon (Fe-N-C) single-atom materials have emerged as the most promising catalysts for the oxygen reduction reaction (ORR), which yet suffers from inadequate stability arising from the attack of ·OH and HO 2 · radicals generated by H 2 O 2 . In this study, density functional theory (DFT) calculations reveal that the presence of peripheral S atoms can regulate the electronic structure of the Fe center and suppress the formation of H 2 O 2 to enhance the catalyst's durability. Thereafter, atomic Fe-N 4 with peripheral S doping is intricately engineered in defect-rich porous carbon nanoshells (Fe-NS-C) through an adsorption-pyrolysis method. The incorporation of S not only optimizes the coordination microenvironment of Fe-N 4 but also induces a larger specific surface area and richer defects. The Fe-NS-C catalyst displays remarkable ORR performance, featuring a half-wave potential (E 1/2 ) of 0.90 V. Its low H 2 O 2 yield (below 1.1 %) and excellent stability (10 mV day in E 1/2 after 10,000 cycles) further underscore the superiority of Fe-NS-C. When employed as the cathode for Zn-air battery, Fe-NS-C achieves an impressive peak power density of 230.1 mW cm −2 and stable charge/discharge potentials over an extended duration of 150 h. This study presents an effective strategy for engineering efficient and durable single-atom electrocatalysts for ORR and Zn-air batteries.
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ELECTROCHIMICA ACTA
·
2024
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IF 5.5
Xiaofei Lei,Wenjuan Li,Kanjun Sun,Sitong Liu,Aoji Liang,Hui Peng,Guofu Ma
Transition metal sulfides embedded in co-doped porous carbon materials with nitrogen and sulfur are a promising catalyst that can effectively solve the problem of slow oxygen reduction reaction (ORR) kinetics. However, monometallic sulfides consisting of a single active component only have monofunctional catalytic activity and cannot effectively increase the rate of oxygen evolution reaction (OER), thus limiting the energy conversion efficiency of Zn-air batteries (ZAB). Herein, a unique silica template assisted in situ pyrolysis strategy is used to synthesize iron (Fe)-doped cobalt sulfide (Co 9 S 8 ) nanoparticle embedded in a honeycomb nitrogen (N), sulphur (S) co-doped porous carbon (Fe/Co 9 S 8 @NSC) electrocatalyst. The introduction of Fe increases the active component of the catalyst and further enhances the catalytic ability of Co 9 S 8 by optimizing the electronic structure through charge transfer effect. Therefore, the rich active sites of Fe/Co 9 S 8 nanoparticles anchored in N, S co-doped carbon materials with rich pore structure enable the catalysts to have good bifunctional catalytic activities of ORR and OER. In particular, the Fe/Co 9 S 8 @NSC has a high half-wave potential of 0.82 V for catalytic ORR and only needs low overpotential of 332 mV at a current density of 10 mA cm −2 for catalytic OER. In addition, the Fe/Co 9 S 8 @NSC catalyst based rechargeable ZAB also exhibits a significant specific capacity of 734 mAh g −1 and prolonged stability of 270 h, which outperforms the bulk of recently reported catalysts based on transition metal sulfides-based catalysts. This research offers a workable method for producing metal sulfides catalysts with bifunctional catalytic activity.
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Journal of Materials Chemistry A
·
2024
·
IF 10.7
Jin Yang,Jun Shi,Yupeng Wu,Huimin Liu,Zhiqiang Liu,Qinwen You,Xinxin Li,Linchuan Cong,Debo Liu,Fangbing Liu,Yue Jiang,Nan Lin,Wenli Zhang,Haibo Lin
Efficient, low-cost cathode catalysts featuring highly dispersed, active sites are pivotal for advancing metal–air batteries. In this study, a bifunctional catalyst was developed using rice husk-based porous carbon (RHPC) with a hierarchical porous structure, comprising a multilayer heterostructure integrating nanoscale CoFe@(Co0.5Fe0.5)S wrapped with nitrogen-doped carbon nanotubes (NCNTs). XRD and TEM images reveal the formation of a CoFe alloy on the RHPC surface and pores, catalyzing the growth of uniform-diameter NCNTs. XPS analysis demonstrates an electron-donating effect on the surface pyridinic-N structure upon introducing the sulfide intermediate layer. Theoretical simulations substantiate these discoveries, emphasizing diminished adsorption of *OH and *OOH, substantially reducing overpotentials for both the ORR by 21 mV and OER by 46 mV compared to CoFe@NCNT/RHPC lacking the sulfur element. This results in CoFe@(Co0.5Fe0.5)S@NCNT/RHPC emerging as an exceptionally effective bifunctional catalyst (ΔE = 0.614 V). Integration into a rechargeable zinc–air battery showcases a peak power density of 136.0 mW cm−2. The unique morphology design and electronic structure optimization significantly improve the catalytic performance.
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ChemSusChem
·
2024
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IF 7.5
Xin Tian,Mengnan Xu,Xin Ma,Guanyu Mu,Junwu Xiao,Shuai Wang
Graphical The 3D Co-based/graphene composite framework, prepared by spontaneous assembly, serves as the template and sources of Co and O.The as-formed Co-Nx sites, along with the Co/CoO nanoparticles and N-doped carbon nanosheets, synergistically function as the active sites to boost the electrocatalytic activity of the oxygen redox reaction. The Co/CoO-NG exhibits a low potential gap (ΔE=0.784 V) for ORR/OER. Reasonable design of low-cost, high-efficiency and stable bifunctional oxygen electrocatalysts is of great significance to improve the reaction efficiency of Zn-air batteries, which is still a huge challenge. Here, we report a highly efficient bifunctional oxygen electrocatalyst with three-dimensional (3D) N-doped graphene network-supported cobalt and cobalt oxide nanoparticles (Co/CoO-NG), which can be in situ synthesized by inducing metal ions on metal plates via graphene oxide as an inducer. This 3D network structure and open active center show excellent bifunctional oxygen electrocatalytic activity under alkaline conditions, and can be used as an air electrode in rechargeable Zn-air batteries, with significantly better power density (244.28 mW cm −2 ) and stability (over 340 h) than commercial Pt/C+RuO 2 mixtures. This work is conducive to advancing the practical application of graphene-based materials as air electrodes for rechargeable zinc-air batteries.
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PubMed
高影响因子
JOURNAL OF AGRICULTURAL AND FOOD CHEMISTRY
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2025
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IF 6.2
Chunhua Li,Zhehang Tian,Guanqun Luan,Luqian Bao,Mengyao Cui,Yixin Ji,Xieyang Zhang
The extensive use of tetracyclines in livestock poses health risks due to their residues in animal-derived food; therefore, developing simple detection methods to replace complex traditional approaches is of paramount importance. Here, we developed a dual-ligand zinc-based metal–organic framework material, Zn-BTC-BDC-NH2 (denoted as ZTD), for the detection of tetracyclines. The intrinsic blue fluorescence of ZTD was quenched upon the introduction of tetracyclines due to electron transfer from −NH2 of ZTD to −CO– and −OH groups of tetracycline molecules; meanwhile, the new green fluorescence emission was generated through π–π stacking between aromatic rings and the formation of complexes between Zn2+ and C–O/C═O groups. In real food samples, ZTD exhibited recovery rates ranging from 93.62 to 110.66%, with detection limits as low as 0.011 μmol·L–1. Additionally, a ZTD fluorescence test paper was developed for portable detection. This study presents a novel tetracycline detection method, offering insights into multiligand metal–organic framework preparation and future sensing method design.
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PubMed
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CATALYSIS TODAY
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2024
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IF 5.2
Longyu Wang,Na Wang,Suohe Yang,Guangxiang He,Haiyan Liu,Xianghai Meng,Chunming Xu,Zhichang Liu,Haibo Jin
A diverse suite of Zn-SAPO-34 catalysts was synthesized employing three distinct methodologies for the incorporation of zinc species: thermal ion exchange, wet impregnation, and physical mixing. The catalysts were characterized using various analytical techniques including XRD, FT-IR, BET, SEM, XRF, XPS, NH 3 -TPD, and Py-IR, to elucidate the crystal structure, morphology, surface acidity, and the presence of zinc species within the catalysts. The study showed that the method of zinc introduction markedly impacts the physicochemical properties of the catalysts. Different approaches to introducing zinc species significantly influence the acid strength and type on the catalyst surface, with variations in the existing states of zinc across the catalysts. Specifically, zinc species introduced via thermal ion exchange coexist as ZnOH + and ZnO within the catalyst, whereas those from wet impregnation and physical mixing are individually present as either ZnOH + or ZnO. Furthermore, the study examined the catalytic performance of these Zn-SAPO-34 catalysts in the dehydration of fructose to produce 5-hydroxymethylfurfural (HMF). Catalysts prepared via thermal ion exchange exhinited superior performance, achieving an remarkable HMF yield of 94.6 %. Additionally, in situ infrared technology was used to investigate the effect of zinc species introduction on the fructose dehydration process, indicating suggesting that the introduction of zinc species enhances the transformation of fructose molecules.
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Asia-Pacific Journal of Chemical Engineering
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2024
·
IF 1.4
Guihua Yang,Jiali Chen,Linxue Yang,Rui Wang
Cu-based catalysts applied in ethynylation reaction of formaldehyde for 1,4-butynediol synthesis has been widely concerned. The activity and stability of Cu-based catalyst is still a challenging task in this field. Here, Cu–Zn catalysts derived from ZIF-8 are prepared by a coprecipitation method and applied in ethynylation reaction of formaldehyde. All catalysts were characterized through thermogravimetric, x-ray diffraction, N 2 physical adsorption–desorption, transmission electron microscopy, H 2 -temperture-programmed reduction, x-ray photoelectron spectroscopy, and Raman and Fourier transform infrared analysis. The effect of calcination temperature of ZIF-8 on the catalyst structures and ethynylation performances are all investigated. The results show that CuO 5h -ZnO 400 catalyst has the best catalytic activity, with a formaldehyde conversion of 98% and 1,4-butynediol selectivity of 100%. It is mainly due to the presence of highly dispersed and small particle CuO. Moreover, CuO 3h -ZnO 400 catalyst prepared by optimized conditions can further improve the stability in ethynylation reaction due to more carbon species on the surface of ZnO. The more carbon contents in Cu–Zn catalyst contribute to the ethynylation activity and stability due to the interaction between Cu and C species favoring Cu 2 C 2 formed. In addition, the ethynylation reaction mechanism catalyzed by Cu–Zn catalyst is illustrated carefully. The Cu–Zn catalysts derived from ZIF-8 can provide some ideas for the application in ethynylation reaction of formaldehyde for 1,4-butynediol synthesis.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Yuanxi Guo,Xinxin Zhang,Hehe Wei,Hai-tao Yu,Ying Xie
High-entropy oxides (HEOs) exhibit excellent structural stability, and the synergistic effects among their constituent elements contribute to performance enhancement, providing vast opportunities for designing novel and efficient electrocatalysts. Utilizing four common transition metals such as Fe, Co, Ni, and Cr as the base and introducing a fifth metal, M (M = Mg, Mn, Zn, and Cu), with different outer electron shells, relevant high-entropy oxides with varying sizes were successfully synthesized via the hydrothermal method. Among all considered samples, FCNCMg, with the smallest particle size, possessed a much larger specific surface area, leading to the exposure of more active sites and thus favoring an improvement of the OER performance. The introduction of the fifth metal induced a redistribution of charges among Fe, Co, Ni, and Cr within the catalyst, resulting in different oxidation states for these metals. Mg addition led the XPS peaks of Fe/Ni and Cr/Co elements to shift towards lower and higher binding energies, respectively. This dynamic compensation effect between metal ions synergistically promoted their OER performance. In alkaline environments, FCNCMg exhibited the best OER performance, with an overpotential of 278 mV at 10 mA cm −2 and a Tafel slope of 49.90 mV dec −1 . Moreover, it demonstrated excellent stability, achieving 50 h at 10 mA cm −2 and 20 h at 50 mA cm −2 . This study, by controlling the composition of HEOs, explored the impact of particle size and synergistic effects on their performance, offering new insights for design and optimization of relevant high-performance HEOs.
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CERAMICS INTERNATIONAL
·
2025
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IF 5.6
Fanlin Kong,Yi liu,Shiyu Cao,Huimin Chen,Yanwei Fan,Junhua Wang,Jincheng Yao,Aimin Chang
In this study, single-phase high-entropy ceramics (HECs) with the composition (Co,Mn,Fe,Zn,Ni,Mg,Al,Cr) 3 O 4 were successfully synthesized using five different types of spinel raw materials. The resulting material demonstrates excellent performance in the negative temperature coefficient (NTC) thermistor field. X-ray diffraction (XRD) analysis confirmed the structure as a cubic spinel with a single Fd-3m space group. The electron microscope image reveals the growth of ceramic grains with increasing sintering temperature, with a uniform distribution of all elements. After 1800 h of accelerated aging at 150 °C, the Δ R / R 0 value was only 0.41 %, indicating the ceramic's exceptional structural stability. X-ray photoelectron spectroscopy(XPS) analysis reveals that electrical conductivity are mainly governed by electron hopping between Mn 3+ and Mn 4+ ions in the octahedral sublattice sites. Impedance spectroscopy further shows that grain boundary resistance is the dominant contributor to the total resistance. This study provides new insights into the synthesis of single-phase HECs materials and proposes strategies to enhance material stability for future applications.
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GREEN CHEMISTRY
·
2024
·Vol. 26
·期 10
·6131-6138
·
IF 9.3
Yan Wang,Xuan Wang,Yonghao Dong,Mingli Peng,Lina Guo,Mengyao Cui,Yuan He,Jiabao Yi,Huijun Ma,Huan Zhang,Haiming Fan
The selective oxidation of alcohols has drawn significant attention in heterogeneous catalysis with the increasing use of Pickering interfacial catalysis (PIC) for green transformations of alcohols. However, it is still highly desirable to design and develop a solid catalyst with easy separation and recycling, made from abundant resources through a simple synthesis route, for the selective oxidation of alcohols. In this study, ferrite nanoparticles, synthesized via a hydrothermal process, were employed to act as a stabilizer and catalyst in PIC for the oxidation of benzyl alcohol using H2O2. The ferrite nanoparticles exhibited higher catalytic performance in PIC than in acetonitrile. The turnover number (TON) of the nanocatalyst in PIC was found to be 1.5–4 times higher than that in acetonitrile, and the reaction constant in PIC (kPIC = 0.712 h−1) was almost twice that in acetonitrile (kCH3CN = 0.310 h−1) for MnFe2O4 nanoparticles. Moreover, other alcohols could also be oxidized with moderately high conversion and selectivity in PIC. Significantly, the ferrite nanocatalyst could be easily separated from PIC using a magnet for reuse, achieving 88% BzOH conversion after five cycles. The use of hazardous organic solvents was avoided in PIC, making it a more advanced, green and sustainable reaction system.
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JOURNAL OF SOLID STATE CHEMISTRY
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2025
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IF 3.5
Jiao Men,Zhuo Dong,Yushan Li,Xiaoying Xie,Chenxi Zhang,Yanhong Qiao,Jingbo Zhang
Vacuum ultraviolet (VUV) with a wavelength of 172 nm was employed to prepare amorphous Zn-doped TiO 2 (ZTO) thin films using titanium tetraisopropoxide as a precursor to form TiO 2 and zinc(II) dibutyldithiocarbamate as a Zn doping source. During the VUV irradiation on the precursor films, the incorporation of zinc and the departure of nitrogen and sulfur enhance the conductivity and electron mobility of the thin films. The prepared ZTO thin films were used as the electron transport layer to fabricate mesoporous perovskite solar cells (PSCs). The optimal doping molar ratio of zinc was determined to be 2 % according to the photoelectric performance of PSCs based on the ZTO thin films. The improved interfacial contact between the ZTO electron transport layer and the electrode substrate reduces the interfacial charge transfer resistance. The synergistic effect of ZTO electron transport layer enhances the power conversion efficiency (PCE) of PSCs from 18.28 % to 21.21 %. In addition, the ZTO thin film was used as the compact layer in quantum dot-sensitized solar cells, significantly improving their performance. Therefore, the VUV irradiation technique is a general method to prepare the doping metal oxide thin films for fabricating high efficiency solar cells with the compact thin film structure.
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