JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xiaoyun Zhang,Fan Yang,Siyuan Sun,Kexin Wei,Hongchen Liu,Guohua Li,Yang Sun,Xi Li,Jinxiu Qian,Shaoxiong Du,Mingjie Li,Yi Lu,Chuangui Xia,Sai Che,Yongfeng Li
An electrocatalyst of single-atomic Mn sites with MnP nanoparticles (NPs) on N, P co-doped carbon substrate was constructed to enhance the catalytic activity of oxygen reduction reaction (ORR) through one-pot in situ doping-phosphatization strategy. The optimized MnSA-MnP-980℃ catalyst exhibits an excellent ORR activity in KOH electrolyte with a half-wave potential (E 1/2 ) of 0.88 V (vs. RHE), and the ORR current density of MnSA-MnP-980℃ maintained 97.9 % for over 25000 s chronoamperometric i-t measurement. When using as the cathode, the MnSA-MnP-980℃ displays a peak power density of 51 mW cm −2 in Zinc-Air batteries, which observably outperformed commercial Pt/C (20 wt%). The X-ray photoelectron spectroscopy reveal that the doped P atoms with a strong electron-donating effectively enhances electron cloud density of Mn SAs sites, facilitating the adsorption of O 2 molecules. Meanwhile, the introduction of MnP NPs can regulate the electronic structure of Mn SAs sites, making Mn SAs active sites exist in a low oxidation state and are less positively charged, which can supply electrons for ORR process to narrow the adsorption energy barrier of ORR intermediates. This work constructs novel active sites with excellent ORR properties and provides valuable reference for the development of practical application.
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CRYSTENGCOMM
·
2023
·Vol. 25
·期 46
·6424-6433
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IF 3.1
Ya-Ping Li,Jian-Hua Zhang,Xiao-Xia Zhang,Sui-Jun Liu
A new Zn(II) metal–organic framework (MOF) with the formula [Zn(BBIP)(2,6-NDC)]n (JXUST-44, BBIP = 3,5-bis(1H-benzo[d]imidazol-1-yl)pyridine and 2,6-H2NDC = 2,6-naphthalic acid) was synthesized under solvothermal conditions. The adjacent Zn(II) ions are connected by BBIP ligands to form one-dimensional (1D) chains, which are further linked by carboxylate groups of 2,6-NDC2− ligands to obtain a two-dimensional layer structure, resulting in a 2D → 3D polycatenated MOF. JXUST-44 can be simplified as a 4-connected sql topology and shows good chemical stability in a wide pH range from 2 to 12 at room temperature. The fluorescence experiments indicate that JXUST-44 presents sensitive and selective detection of salicylaldehyde (SA), acetylacetone (acac) and H2PO4− with the detection limits of 0.074, 10.311 and 0.011 ppm, respectively. It is worth noting that JXUST-44 shows turn-on fluorescence toward acac and H2PO4−, as well as good recyclability and stability for acac, SA and H2PO4−. Therefore, JXUST-44 can be considered as a good fluorescent sensor for acac, SA and H2PO4−. The sensing mechanism has also been studied in detail.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Chao Chen,Shilong Zhou,Jiawei Xia,Le Li,Xingyue Qian,Fengxiang Yin,Guangyu He,Haiqun Chen
Exploring efficient, easy-to-manufacture, and inexpensive bifunctional electrocatalysts with abundant accessible active sites is crucial for rechargeable zinc-air batteries (ZABs). Herein, we report the strategy consisting of the space confinement and pore-making engineering to fabricate single-atom catalyst enriched with Fe-N 4 sites anchored on N -doped hierarchically porous carbon (Fe-NC-C 3 N 4 ). The optimized Fe-NC-C 3 N 4 exhibits excellent oxygen reduction/evolution reaction (ORR/OER) activities with a half-wave potential ( E 1/2 ) of 0.90 V vs. RHE and a promising low overpotential of 0.305 V vs . RHE at 10 mA·cm −2 in alkaline electrolyte. These superior catalytic activities are attributed to the combined effect between the atomic active sites and the well-balanced micro-meso-macropore structures. The homemade liquid Zn-air battery (ZAB) assembled with Fe-NC-C 3 N 4 catalyst displays a power density of 133.59 mW·cm −2 and a significant energy density of 882.58 mAh·g −1 , exceeding those of the equipment with commercial Pt/C-RuO 2 (56.82 mW·cm −2 and 643.87 mAh·g −1 , respectively). Particularly, the corresponding flexible wearable ZAB manifests outstanding foldability and cyclical stability. This work opens a new perspective for the structural design of single-atom catalysts in the energy storage and conversion area.
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Food Bioscience
·
2023
·
IF 5.2
Wenqing Li,Jinting Zhu,Xinru Qi,Changyan Sun,Wenjun Li,Zhidong Chang
Gossypol is a poisonous substance in cottonseed which seriously harms the internal organs, blood vessels, nerves, and reproductive systems of organisms. Therefore, detecting gossypol is of great significance in the field of food safety. This manuscript constructs a novel target-oriented gossypol fluorescence probe based on the energy competition absorption mechanism. The probe is a zinc-based metal organic framework material (Zn-MOF) with blue fluorescence, which can achieve rapid and sensitive detection of gossypol through fluorescence “turn-off” effect. It has the advantages of low detection limit (16.6 nM), ultra-fast response time (8 s), and favorable selectivity. Interestingly, this probe can be reused and the fluorescence can still be recovered after five cycles when detecting gossypol. In addition, the application of the fluorescent probe in cottonseed oil and fetal bovine serum is reliable, with the recovery of 99.35%–101.5% and the relative standard deviation of less than 2.72%. These results indicate that the developed sensor has prominent application potential in the field of food and biological detection.
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Nano Research
·
2023
·
IF 9.9
Chen Yan,Yang Zhenrui,Wang Juan,Yang Yun,He Xuedong,Wang Yang,Chen Jiadong,Guo Yaqing,Wang Xin,Wang Shun,Jin Huile
Enhancing catalytic activity through modulating the interaction between N-doped carbon and metal phosphides clusters is an effective approach. Herein, the electronic structure modulation of CoP 2 supported N-modified carbon (CoP 2 /NC) has been designed and prepared as efficient electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER), and hydrogen evolution reaction (HER). Notably, CoP 2 /NC-1 catalyst exhibits impressive performance in alkaline media, with an ORR half-wave potential of 0.84 V, as well as OER and HER overpotentials of 290 and 129 mV (at 10 mA·cm −2 ), respectively. In addition, CoP 2 /NC-1 produces a power density as high as 172.9 mW·cm −2 , and excellent reversibility of 100 h at 20 mA·cm −2 in home-made Zn-air batteries. The experimental results demonstrate that the synergistic interactions between N modified carbon substrate and CoP 2 material significantly enhance the kinetics of ORR, OER, and HER. Density functional theory (DFT) calculations reveal the strong electrons redistribution of CoP 2 induced by high-density N atoms at the interface, thus optimizing the key intermediates and significantly lower the energy barrier of reactions. These electronic adjustments of CoP 2 greatly enhance its kinetics of ORR/OER/HER, leading to faster reactions. This study provides profound insights into the specific modification of CoP 2 by N-doped carbon, enabling the construction of efficient catalysts.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 15
·9761-9770
·
IF 12.732
Dan Wang,Hao Xu,Peixia Yang,Lihui Xiao,Lei Du,Xiangyu Lu,Ruopeng Li,Jinqiu Zhang,Maozhong An
Extensive efforts have been devoted to active site designing for non-precious metal electrocatalysts; however, the porous structure engineering has been less emphasized, particularly for catalysts for gas diffusion electrodes, e.g., the cathode (oxygen reduction reaction, ORR) of Zn–air batteries. The desired porous structure is not only important for exposing high-density active sites but also beneficial for boosting mass transfer. Here, a dual-template strategy is proposed for constructing hierarchically porous structural Fe–N–C catalysts with dense active Fe–Nx moieties for the cathode of Zn–air batteries. The dual ZnCl2 and MgO hard templates jointly promote the formation of hierarchically interconnected carbon networks. The experimental results indicated both significantly improved active site accessibility and mass transfer, reasonably leading to enhanced ORR activity in conventional three-electrode cells. Particularly, it is deduced that the microporous structure is beneficial for dense active Fe–Nx moieties, while the ultra-macroporous structure is conducive to mass transfer during the ORR process. We further applied this dual-template-mediated catalyst in a real-world liquid Zn–air battery, which presents a high open-circuit voltage of 1.48 V and a remarkable energy density of 952.8 W h kgZn−1. Such robust battery performance is among the best compared with reported Zn–air batteries using non-precious metal catalysts. Particularly, a peak power density of 116.8 mW cm−2 is achieved in an all-solid-state Zn–air battery.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Guangyao Zhai,Yuanyuan Liu,Yuyin Mao,Honggang Zhang,Lingtong Lin,Yujie Li,Zeyan Wang,Hefeng Cheng,Peng Wang,Zhaoke Zheng,Ying Dai,Baibiao Huang
CO 2 cycloaddition reaction from propylene oxide and CO 2 to cyclic carbonates is a desirable process to become carbon neutral. Photo energy can decrease the temperature and pressure needed for this reaction according to our previous results. However, the relationship between Lewis acidity and the photophysical process needs to be clarified and optimized. Hence, in this work, Zn is introduced into UiO-bpydc via the coordination of Zn with the bipyridyl group in bpydc. It is found that the introduction of Zn not only effectively activate propylene oxide, but also promote ligand to metal charge transfer (LMCT) process, which ultimately is beneficial for CO 2 activation. However, Ce plays a negative effect under light irradiation. namely, the presence of Ce facilitates the energy transfer process rather than the LMCT process.
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CRYSTENGCOMM
·
2021
·Vol. 23
·期 39
·6899-6908
·
IF 3.545
Huimin Wang,Tingting Wang,Zibin Huang,Yizhuo Liu,Dehui Leng,Junli Wang
The growth of metal chalcogenide nanowires (NWs) on metal substrates is challenging work since the direct reactions taking place between the chalcogen (S, Se or Te) and zero-valent metal (M0) are frequently unable to regulate the crystallization of nanocrystals in an anisotropic one-dimensional (1D) manner. We here report the use of Ag2Se seeds as catalyst particles to realize the growth of metal selenide (MSe) NWs on their respective metal foil or flakes, including ZnSe/Zn, CdSe/Cd, and MnSe/Mn material systems. Metal foil or flakes (M = Zn, Cd and Mn) serve as a support substrate as well as a metal cation source during the NW synthesis. The preformed Ag2Se seeds play the roles of not only catalytic particles that initiate a so-called solution–solid–solid process to produce crystalline MSe NWs on metal substrates, but also inert impurities that promote an electrochemical anodic reaction of the metal to supply metal cations (M0 − 2e → M2+) for the NW formation. The microstructural studies by HRTEM reveal the polytypism and particularly the diameter-dependence of crystal phases and growth directions in the resulting MSe NWs, which can be rationalized from the viewpoints of the energetics and the catalyst/NW interfacial structures. These semiconductor NWs grown on metal foil or flakes may find wide use in photoelectric catalysis and devices without a transfer process of free-standing NWs onto a conductive support substrate.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2021
·
IF 5.316
Manlin Zhu,Wangfeng Cai,Hongbo Wang,Leqiu He,Yan Wang
A morphologically adjustable metal-organic framework (MOF) template and a unique hierarchical structure show improved electrochemical performance of electrode materials for supercapacitors . Herein, Zn/Co-MOF-derived zinc-cobalt oxide/nickel cobalt layered double hydroxides (Zn-Co-O/NiCo-LDH) hierarchical core/shell nanostructures on nickel foam (NF) were synthesized by simple methods and exhibited high specific capacitance. The results showed that both the reasonable morphology of the MOF-templated continuous nanosheet network and synergy between transition bimetallic oxides and transition bimetallic hydroxide played an important role in improving the electrochemical properties . Hence, the as-prepared Zn-Co-O/NiCo-LDH battery-type electrode exhibited excellent specific capacitance of 2275.2 F/g at 1 A/g and remarkable cycling stability of 82.4% capacitance retention after 5000 cycles. Moreover, the as-prepared Zn-Co-O/NiCo-LDH was used as the positive electrode to assemble a hybrid supercapacitor (HSC) device, which attained a distinguished energy density of 44.5 W h/kg at a power density of 800 W/kg and satisfactory stability (71.5% retention after 5000 cycles). It was concluded that MOF-templated core/shell heterostructures in electrode materials have broad prospects and great potential for energy storage.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yingjie Chen,Chong Gong,Zhihao Shi,Di Chen,Xing Chen,Qian Zhang,Beili Pang,Jianguang Feng,Liyan Yu,Lifeng Dong
A melt-salt-assisted method is utilized to construct an onion-like hybrid with Co/CoO nanoparticles embedded in graphitic Fe-N-doped carbon shells (Co/CoO@FeNC) as a bifunctional electrocatalyst. The iron-polypyrrole (Fe-PPy) is firstly prepared with a reverse emulsion. Direct pyrolysis of Fe-PPy yields turbostratic Fe-N-doped carbon (FeNC) with excellent oxygen reduction reaction (ORR) electrocatalysis, while the melt salt (CoCl 2 ) mediated pyrolysis of Fe-PPy obtains onion-like Co/CoO@FeNC with a reversible overvoltage value of 0.695 V, largely superior to Pt/C and IrO 2 (0.771 V) and other Co-based catalysts reported so far. The ORR activity is mainly due to the graphitic FeNC and further enhanced by Co N x bonds, whereas the oxygen evolution reaction (OER) activity is principally due to the Co/CoO composite. Concurrently, Co/CoO@FeNC as cathode catalyst enables Zn-air battery with a high open circuit voltage of 1.42 V, a peak power density of 132.8 mW cm −2 , a specific capacity of 813 mAh g Zn −1 , and long-term stability.
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ELECTROCHIMICA ACTA
·
2020
·
IF 6.215
Denian Li,Huibing Chen,Yuyuan Zhang,Jizhang Yang,Haoran Yuan,Yong Chen
With quite limited use, biomass tar has been a long-standing issue that strongly impaired the cost-efficiency of biomass gasification. Here, a facile activation-annealing route for upcycling biomass tar into graphene nanohybrids with developed porosity and enriched pyridinic nitrogen was reported, whilst the metal-free product revealed with superior catalytic activities to the benchmark Pt/C and RuO 2 catalysts toward oxygen reduction reaction (ORR) and evolution reaction (OER). By associating the dual functionalities with products’ physiochemical properties, it was unveiled that those pyridinic-N and defects were accounted for the promoted oxygen reduction and evolution, respectively. Together with reinforced electric conductivity and hierarchical porosity and enlarged interface via ammonia annealing, the heterogeneously structured carbon catalyst finally endowed an assembled primary Zn-air battery with maximum energy density of 121 mW/cm −2 , in addition to robust stability against long-term running. This work highlights the great potential of biomass tar for advanced carbon materials , and therefore a novel strategy to address the tar-related challenges faced by gasification technologies.
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ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Yuanyuan Hu,Ping Shen,Na Zeng,Lulu Wang,Di Yan,Lulu Cui,Kai Yang,Cuiping Zhai
Multifunctional metal–organic supramolecular hydrogels have achieved great progress nowadays. However, their applications in aqueous batteries for flexible energy storage devices remain limited due to their unsatisfactory mechanical properties. Here, we report a rapid formation of supramolecular hydrogel by adenosine 5′-monophosphate (AMP) and manganese ions (Mn2+). Additionally, the AMP–Mn hydrogel is combined with chemical cross-linking poly(vinyl alcohol) (PVA) polymer networks to form an AMP–Mn/PVA hybrid hydrogel, which effectively solves the problems with regard to the mechanical properties and stability of metal–organic supramolecular hydrogels as well as self-healing of tough chemical cross-linking polymer networks. The AMP–Mn/PVA hybrid hydrogel served as the hydrogel electrolyte to fabricate flexible Zn–MnO2 batteries, which exhibit fast ion conductivity, excellent electrochemical stability, and robust mechanical strength, indicating feasible practical application prospects. This investigation provides a promising opportunity for the application of metal–organic supramolecular hydrogels in the field of energy storage.
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