Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 19
·9981-9990
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IF 11.301
Cheng Du,Yijing Gao,Jianguo Wang,Wei Chen
Single-atom catalysts (SACs) provide the most efficient metal utilization for various catalytic reactions. Meanwhile, hierarchical pore structures play a decisive role in determining the catalytic activity of N-doped porous carbon materials, since normally micropores provide active locations and macro/mesopores serve as mass transport channels. However, it remains challenging to engineer highly dispersed SACs with hierarchical pore structures due to the complexity in synthesizing extra templates with controlled sizes and the possible exogenous impurities from templates. Herein, we develop a facile “confined recrystallization” self-template strategy to synthesize a hierarchical porous Fe SAC on N-doped carbon (Fe-NC SAC) with an iron mass loading of 1.5 wt%, by using polyvinylpyrrolidone (PVP), ferric nitrate and melamine. In this novel strategy, the introduced PVP can restrict the recrystallization of ferric nitrate owing to its large molecular weight. The formed nano-sized ferric nitrate crystals can not only serve as multifunctional self-templates to produce hierarchical pores, but also form atomically dispersed Fe–Nx sites through getting nitrogen from melamine. With the Fe-NC SAC as the catalyst, an excellent bifunctional ORR/OER performance and long-term durability superior to those of Pt/C and RuO2 are achieved in both liquid and solid Zn–air battery tests. Notably, in the flexible solid Zn–air battery, the Fe-NC SAC showed a high discharge voltage of 1.25 V and stable charge–discharge cycling at 1 mA cm−2 under different bending conditions. Further density functional theory (DFT) calculations showed that the ORR follows the association mechanism of O2 → *OOH → *O → *OH → OH−, while the OER goes on through the mechanism of OH− → *OH− → *O → *OOH → O2, with a low theoretical overpotential of 1.21 V on the Fe-NC SAC. This work not only provides a novel strategy to endow SACs with a hierarchical pore structure, but also represents an example of how to effectively investigate the correlation between the structure and catalytic activity of catalysts.
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COMPOSITES PART B-ENGINEERING
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2020
·
IF 7.635
Xiuyun Yao,Jiajia Li,Yajing Zhu,Ling Li,Wenming Zhang
Here, we successfully synthesize three-dimensional (3D) callistemon-like hierarchical networks structural catalysts (CoNC/NCNTs@CNF) in which Co nanoparticles are encapsulated within N-doped carbon nanotubes apexes via electrospinning method combined with two-step pyrolysis process . Benefiting from the unique 3D callistemon-like structure, CoNC/NCNTs@CNF affords adequate surface area (261 m 2 g −1 ) and the enhanced electronic conductivity (even superior to Pt/C and RuO 2 ). Due to the synergistic effect of the coupling between highly Co–N–C active sites and unique 3D callistemon-like structure, CoNC/NCNTs@CNF was explored as the trifunctional electrocatalysts for oxygen reduction reaction , oxygen evolution reaction , and hydrogen evolution reaction . Further, we assemble the catalysts as an air electrode for Zn-air batteries, demonstrating a maximum power density of 260 mW cm −2 , and excellent cycling stability even after 43 h at 5 mA cm −2 . Thus, this work offers a guide to the design of metal organic frameworks-derived 3D structure materials combined with electrospinning for wider application in renewable energy technologies .
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RSC Advances
·
2021
·Vol. 11
·期 36
·21991-21999
·
IF 3.361
Kaixuan Zhang,Xu Peng,Can Cheng,Yang Zhao,Xixun Yu
In order to solve the problem of aseptic loosening of artificial joints resulting from the wear particles of artificial joint components in total joint replacement (TJR), we synthesized a new kind of metalo-organic particle (Sr/Zn-doped CPP/GNS) using spark plasma sintering (SPS) as a filler to enhance the comprehensive performance of UHMWPE. Sr/Zn-doped CPP/GNS was interfused evenly with UHMWPE particles and cured in a hot press instrument to prepare Sr/Zn-doped CPP/GNS/UHMWPE composites. FTIR and SEM were carried out to characterize Sr/Zn-doped CPP/GNS particles. EDS was carried out to characterize Sr/Zn-doped CPP/GNS/UHMWPE. The micro-structure, hardness, impact strength, tribology and bio-activities of Sr/Zn-doped CPP/GNS/UHMWPE composite materials were also investigated. The results confirmed the effectiveness of this method. The hardness, impact strength, and tribology of the composites were enhanced by adding homodispersed Sr/Zn-doped CPP/GNS particles into UHMWPE. In the meantime, Sr/Zn-doped CPP/GNS/UHMWPE composites could significantly promote the growth of osteoblasts due to the bio-activity of Sr/Zn-doped CPP/GNS. Furthermore, the addition of Sr/Zn-doped CPP/GNS particle-fillers into UHMWPE could promote the secretion of OPG from osteoblasts and inhibit the secretion of RANKL from osteoblasts, and thus increase the OPG/RANKL ratio. All the results above showed that Sr/Zn-doped CPP/GNS/UHMWPE composites with appropriate Sr/Zn-doped CPP/GNS content possessed superior physicochemical performances and bio-properties, and could be considered as promising materials to treat aseptic loosening in total joint replacement.
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PubMed
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Nano Energy
·
2019
·
IF 15.548
Hongling Guan,Shuangyi Zhao,Huaxin Wang,Dongdong Yan,Ming Wang,Zhigang Zang
White light emitting diodes (WLEDs) based on all-inorganic halide (CsPbX 3 , X = Cl, Br and I) perovskite quantum dots (QDs) have attracted broad attention due to their high brightness. However, their poor stability and anion-exchange reaction when utilized together are still the main challenges that impede their applications. Herein, a one-step in situ method under room temperature in air is proposed to synthesize CsPbBr 3 QDs coated with SiO 2 (CsPbBr 3 @SiO 2 ), where the whole process takes only 20 s. The as-prepared CsPbBr 3 @SiO 2 QDs samples present an enhanced stability in the thermal and polar-solvent environment, maintaining its high photoluminescence quantum yield (PLQY~75%). Thereby WLEDs are constructed by combining CsPbBr 3 @SiO 2 with red Ag–In–Zn–S QDs on InGaN blue chip, achieving a high color rendering index (CRI) of 91, a correlated color temperature (CCT) of 3689 K and a power efficiency of 40.6 lm W −1 .
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SENSORS AND ACTUATORS B-CHEMICAL
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2024
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IF 8
Zaihua Duan,Boyu Zhang,Mingxiang Zhang,Zhen Yuan,Yadong Jiang,Huiling Tai
Electrochemical power generation humidity sensors have received great attention recently, but it is challenging for achieving good humidity sensing and power generation performances simultaneously. Herein, we construct a high-performance power generation humidity sensor based on NaCl/sodium alginate (SA) humidity sensing electrolyte and Cu/Zn electrodes. Benefiting from the reasonable selection of humidity sensing electrolyte and electrode materials and the design of sensor structure, the optimized NaCl/SA humidity sensor exhibits wide humidity sensing detection range (10.9−91.5% relative humidity (RH)), short response time (5.6 s), and good repeatability (20 cycles) at 25°C. Importantly, the humidity sensor has high response voltage (∼0.7 V), large short circuit current (∼24 μA) and loading power (∼2.63 μW) at 91.5% RH. The NaCl/SA humidity sensor can be used for passive visual humidity indication by connecting it to a pointer microammeter. In addition, we designed signal processing circuit and software program to recognize respiratory patterns using NaCl/SA humidity sensor. This work not only achieves a high-performance electrochemical humidity sensor, but also provides a useful reference for its applications in passive visual humidity and respiratory patterns detections.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Lu Zhang,Ling-Ling Liu,Jiu-Ju Feng,Ai-Jun Wang
Three-dimensional (3D) hollow carbon is one of advanced nanomaterials widely applied in oxygen reduction reaction (ORR). Herein, iron niobate (FeNb 2 O 6 ) nanoparticles supported on metal-organic frameworks (MOFs)-derived 3D N -doped interconnected open carbon cages (FeNb 2 O 6 /NICC) were prepared by methanol induced assembly and pyrolysis strategy. During the fabrication process, the evaporation of methanol promoted the assembly and cross linkage of ZIF-8, rather than individual particles. The assembled ZIF-8 particles worked as in-situ sacrificial templates, in turn forming hierarchically interconnected open carbon cages after high-temperature pyrolysis. The as-made FeNb 2 O 6 /NICC showed a positive onset potential of 1.09 V and a half-wave potential of 0.88 V for the ORR , outperforming commercial Pt/C under the identical conditions. Later on, the as-built Zn-air battery with the FeNb 2 O 6 /NICC presented a greater power density of 100.6 mW cm −2 and durable long-cycle stability by operating for 200 h. For preparing 3D hollow carbon materials, this synthesis does not require a tedious removal process of template, which is more convenient than traditional method with silica and polystyrene spheres as templates. This work affords an exceptional example of developing 3D N -doped interconnected hollow carbon composites for energy conversion and storage devices.
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PubMed
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FUEL
·
2024
·
IF 6.7
Guosheng Li,Yu Ding,Xiaohan Li,Kunhong Li,Xinrui Yin,Liang Zhao,Shenyong Ren,Chunming Xu,Baojian Shen
Regulation of electronic structure of metal active phase for catalysts has been known as efficient in promoting its catalytic activity; however, manipulating the activity of catalysts via controllable metal active phase electronic structure is still challenging. A non-equilibrium electronic structure Fe-based bulk catalyst has been developed via controllably adding P species, where the non-equilibrium electronic structure of Fe species is formed through the electron transfer from the Zn species through the P electronic channel. As a result, the catalytic activity of the modified Fe-based bulk catalysts has increased by 24.4–50.4%. Meanwhile, the sulfurization degree (SD) of the modified Fe-based bulk catalysts has increased by 5.6–25.9%. In addition, the HDS reaction rate constant ( k HDS ) has increased by about 2.0 times, and the DDS reaction rate constant ( k DDS ) has increased by about 2.4 times. The P modifying can regulate the directional transfer of unpaired free electrons between Fe and Zn species to form a more non-equilibrium electronic structure of Fe species, which can reduce the energy barrier of the C–S bond adsorbed on the P-modified Fe-based bulk catalysts. Importantly, the P species can be used as an active site to adsorb S-containing compounds in the modified Fe-based bulk catalysts, which is conducive to generating more coordinatively unsaturated sites (CUSs). The former can promote the formation of the more non-equilibrium electronic structure of Fe species, and the latter can adjust the adsorption active site of S-containing on the catalyst surface. Therefore, an electron transfer channel is formed among Fe, Zn, and P species, and another one is formed among Fe, P, and S-containing compounds, which form a dual-channel electron transfer behavior. Furthermore, the specific surface area, total pore volume, and reducibility of the modified Fe-based bulk catalysts have also shown varying degrees of improvement via the controllable addition of P species.
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Materials Today Communications
·
2024
·
IF 3.7
Tianlu Li,Aixian Tian,Wei Li,Yun Zhao,Minfang Chen
A one-step hydrothermal method was used to deposit a in situ composite coating on a magnesium alloy by adding ZIF-8 nanoparticles modified by polydopamine (PDA) (PDA@ZIF-8) as a photoabsorbing agent and growing Mg-Al double-layer hydroxide (LDH). The results showed that PDA@ZIF-8 nanoparticles had significant influence on the corrosion resistance, antibacterial properties, and biocompatibility of the LDH coating, and improved the compactness and crystallinity of LDH by regulating the growth of its lamella. Compared with the LDH coating, the corrosion current density of the composite coating by adding PDA@ZIF-8 nanoparticles was reduced from 2.28×10 -5 to 1.86×10 −6 A·cm -2 . And its immersion corrosion rates were 0.89 ± 0.05 mm·year −1 in SBF solution for 8 days. Meanwhile, it had antibacterial efficacy of 99.99% and 99.99% against Escherichia coli and Staphylococcus aureus , respectively, with the in vitro photothermal conversion efficiency of 29.77%. Moreover, besides greatly improving osteogenic activity and biocompatibility in vitro, the composite coating with the addtion of PDA@ZIF-8 nanoparticlescan also drive M1-type macrophages to M2-biased phenotypes after exposure to 808 nm NIR light, changing in macrophage secretion for tissue regeneration, and fulfill the excellent antibacterial properties in vivo antibacterial implantation test. This method can provide an effective way and strategy for regulating and enhancing the antibacterial functionalization and improving the corrosion resistance of the double-layer hydroxide coating on the surface of magnesium alloys.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Jin Wang,Yefei Chen,Wei Cheng,Hong Li,Meng Liu,Xianmang Xu,Peiyu Zhao,Lixiang Xing,Daijie Wang
Carbon based dual-metal sites materials have garnered considerable attention owing to their atomically dispersed active sites and synergistic effects. However, precise control over the coordination environment and prevention of metal aggregation remain challenging. Herein, we demonstrate a green synthesis of Cu-Fe dual atomic clusters on N-doped porous carbon (CuFe AC@NC) via a chitosan-glutamic acid hydrogel platform. The hydrogel’s amino/hydroxyl/carboxyl groups ensure uniform bimetallic dispersion and inhibit pyrolysis-induced aggregation. Combined experimental and theoretical analyses reveal the distinct roles of Cu and Fe: Fe induces catalytic graphitization for hierarchical pores and enhanced ORR activity, while Cu modulates electronic states and prevents Fe aggregation. The optimized CuFe AC@NC exhibits exceptional ORR activity, and enables Zn-air batteries with a high open-circuit voltage (1.470 V), remarkable specific capacity (806.2 mAh g −1 ), and stable cycling performance. This work provides a green methodology for designing dual-metal-site catalysts and elucidates structure–property relationships, advancing the development of cost-effective energy storage systems.
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Small
·
2024
·
IF 13
Mengmeng Zhang,Mingzhu Lu,Yimin Gong,Yannan Yang,Junfei Song,Jianing Li,Zhenxia Chen,Yun Ling,Yaming Zhou
Precise integration of diverse therapeutic approaches into nanomaterials is the key to the development of multimodal synergistic cancer therapy. In this work, tadpole-like carbon nanotubes with Fe nanoparticle encapsulated at the head and Zn single-atom anchored on the body (Fe@CNT-Zn) is precisely designed and facilely prepared via one-pot carbonization. In vitro studies revealed the integration of chemotherapy (CT), chemodynamic therapy (CDT), photothermal therapy (PTT), and photodynamic therapy (PDT) in Fe@CNT-Zn as well as the near-infrared light (NIR)-responsive cascade therapeutic efficacy. Furthermore, in vivo studies demonstrated the NIR-triggered cascade-amplifying synergistic cancer therapy in a B16 tumor-bearing mouse model. The results not only showcased the Fe@CNT-Zn as a potential tetramodal therapeutic platform, but also demonstrated a proof-of-concept on metal–organic framework-based “one stone for multiple birds” strategy for in situ functionalization of carbon materials.
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PubMed
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Chunmei Xu,Mengran Lou,Rui Liu,Taotao Lv,Yang Wang,Ruiying Wang,Hongtao Liu,Xia Kong
Metal-nitrogen-carbon (M–N–C) catalysts are promising alternatives to precious metal-based bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in Zn-air batteries (ZABs). Herein, FeCo@nitrogen doped carbon nanotube/nitrogen doped reduced graphene oxide (FeCo@NCNT/N-rGO) catalyst with unique 3D heterostructure was synthesized through one-step pyrolysis of FeCo-ZIF-8 precursor anchored on graphene oxide (FeCo-ZIF-8/GO). Benefiting from the coupling of FeCo dual-metal sites with nitrogen-doped carbon substrates, the FeCo@NCNT/N-rGO catalyst achieved extraordinary bifunctional oxygen electrocatalytic activity, exhibiting a high ORR half-wave potential (E 1/2 ) of 0.881 V (vs. RHE), which was superior to the Pt/C catalyst (0.838 V), and OER overpotential of 343 mV at 10 mA cm −2 , merely inferior to RuO 2 by 33 mV. The resulting ΔE (defined as E j=10 − E 1/2 ) reaches an impressively low value of 0.69 V, highlighting its superior reversible oxygen electrocatalytic performance. Meanwhile, achieving a high-power density of 240 mW cm −2 and open circuit voltage (OCV) of 1.488 V in ZAB applications, superior to that of Pt/C + RuO 2 in ZAB (1.447 V; 143 mW cm −2 ). Flexible solid-state ZAB with FeCo@NCNT/N-rGO achieves 1.416 V OCV and 47.4 mW cm −2 power density, remaining stable even when bent 180°. This study guides design of dual-site non-precious metal bifunctional oxygen catalysts.
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Journal of Materials Chemistry C
·
2018
·Vol. 6
·期 46
·12566-12574
·
IF 5.976
Xiaohui Li,Lei Zhou,Miroslav D. Dramićanin,Qiang Tang,Xiping Jing,Jianxin Shi,Yiqin Xu,Mingmei Wu
Broad emission with a full and continuous color spectrum realized by crystal engineering is extensively desired to simulate natural sunlight and improve the white color quality. Herein, new insight into the modulation of B site order–disorder and intrinsic oxygen defects for complex perovskite (A3B′B2′′O9) Sr3−xScxZnNb2O9 (0 ≤ x ≤ 0.1) phosphors is demonstrated for broad-band emission via crystal engineering. We elucidate that the spectrum of Sr3ZnNb2O9 synthesized at an optimal temperature exhibits two emission bands under near-ultraviolet excitation (λex = 374 nm) which is readily available from near ultraviolet chips. The two broad emission bands can be ascribed to charge transfer from the empty 4d (t2g)-orbitals of Nb5+ ions to the filled 2p-orbitals of O2− ions and the intrinsic oxygen defects. Further, as a proposed strategy to optimize the luminescence property of Sr3ZnNb2O9 (SZN), we realized A-site nonequivalent doping to induce B-site disordering and cancel the luminescence quenching which results from B site ordering. The A-site nonequivalent doping efficiently offsets intrinsic oxygen defects, as validated by systematic analyses of experiments and DFT calculations. Consequently, the novel phosphor Sr3−xScxZnNb2O9 (x = 0.1) shows a high color rendering index (Ra = 82.2) and negligible color shift. In addition, its emission intensity is enhanced by ∼70 times as compared to the pristine Sr3ZnNb2O9.
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