PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 48
·e2314362120
·
IF 11.1
Fengkai Zuo,Hao Zhang,Yu Ding,Yongshuai Liu,Yuhao Li,Hengjun Liu,Fangchao Gu,Qiang Li,Yaqun Wang,Yue Zhu,Hongsen Li,Guihua Yu
Interfacial catalysis occurs ubiquitously in electrochemical systems, such as batteries, fuel cells, and photocatalytic devices. Frequently, in such a system, the electrode material evolves dynamically at different operating voltages, and this electrochemically driven transformation usually dictates the catalytic reactivity of the material and ultimately the electrochemical performance of the device. Despite the importance of the process, comprehension of the underlying structural and compositional evolutions of the electrode material with direct visualization and quantification is still a significant challenge. In this work, we demonstrate a protocol for studying the dynamic evolution of the electrode material under electrochemical processes by integrating microscopic and spectroscopic analyses, operando magnetometry techniques, and density functional theory calculations. The presented methodology provides a real-time picture of the chemical, physical, and electronic structures of the material and its link to the electrochemical performance. Using Co(OH)2 as a prototype battery electrode and by monitoring the Co metal center under different applied voltages, we show that before a well-known catalytic reaction proceeds, an interfacial storage process occurs at the metallic Co nanoparticles/LiOH interface due to injection of spin-polarized electrons. Subsequently, the metallic Co nanoparticles act as catalytic activation centers and promote LiOH decomposition by transferring these interfacially residing electrons. Most intriguingly, at the LiOH decomposition potential, electronic structure of the metallic Co nanoparticles involving spin-polarized electrons transfer has been shown to exhibit a dynamic variation. This work illustrates a viable approach to access key information inside interfacial catalytic processes and provides useful insights in controlling complex interfaces for wide-ranging electrochemical systems.
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SYNTHETIC METALS
·
2023
·
IF 4.4
Ruiqi Li,Fuqiang Zhai,Yuan Liu,Qiang Wang,Hao Wei,Wencong Wu,Chunhong Zhang,Wenhang Chen
Considering the diverse structures and superior properties of metal-organic frameworks (MOFs), we successfully synthesized Co/NC@PANI composites through high-temperature pyrolysis and in-situ chemical oxidation using zeolitic imidazolate framework compounds (ZIFs) as precursors. The inclusion of polyaniline in the composites improved conductive loss and interfacial polarization, while the porous structure of Co/NC and uniformly dispersed cobalt nanoparticles can contribute to electromagnetic wave multiple reflection and magnetic loss. By synergistically dissipating electromagnetic waves through various loss mechanisms, we were able to control electromagnetic parameters and optimize performance, resulting in the development of Co/NC@PANI composites with exceptional electromagnetic properties. The minimum reflection loss (RL min ) reaches − 46.28 dB at 5.76 GHz, with a matching thickness of 5 mm. And the effective absorption bandwidth (EAB, RL<− 10 dB) reaches 3.52 GHz at a thickness of 2.5 mm. This work provides an efficient enlightenment for constructing microwave-absorbing material with high performance.
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JOURNAL OF DRUG DELIVERY SCIENCE AND TECHNOLOGY
·
2023
·
IF 5
Jicheng Cui,Wenjing Zhao,Jiangtao Wu,Dongmei Zhang,Longguang Liu,Hui Qiao,Zeyu Yan,Yuejun Fu,John F. Trant,Yingqi Li
Combination chemotherapy can slow the emergence of resistance, but can also lead to a significant exacerbation of off-target effects. Mediated drug release can ameliorate this situation: in this study, mitoxantrone (MTO) and doxorubicin (DOX) were co-loaded onto a nanodiamond (ND) scaffold, through physical adsorption, to prepare an ND/MTO/DOX (NMD) nanodrug. The drug loading of MTO and DOX were 119 ± 3 μg mg −1 and 60 ± 3 μg mg −1 , respectively. This NMD exhibits excellent stability with negligible drug leakage upon storage. The NMD nanoparticles enter cells via the clathrin and caveolae co-mediated endocytosis pathways and primarily remain within the lysosomes. Cytotoxicity tests showed that the NMD has an enhanced synergistic effect compared with an ND loaded with either drug alone, and has a slow but effective rate of drug release. Intraperitoneal injection of the NMD-drug into tumor-bearing mice demonstrated that the NMD rapidly localizes to the tumor site with very limited dispersion to other organs. The NMD strongly suppressed tumor growth in vivo with significantly reduced toxic side effects compared to mice treated with the free drugs. These results suggest that the as-prepared NMD has potential clinical applications for the targeted co-delivery of multiple chemotherapeutics.
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EUROPEAN POLYMER JOURNAL
·
2023
·
IF 6
Wanyu Zhang,Weiping Chen,Jiamin Lv,Ying Wu,Xinwu Ba,Liping Fang
Multi-responsive hydrogels for temperature sensor and information encryption were developed through the synergistic application of light, temperature and pH response of the hydrogel. The multi-responsive hydrogels were prepared by copolymerization of dimethylaminoethyl methacrylate (DMAEMA) and 7-(2-methacryloyloxyethoxy)-4-methylcoumarin (CoumMAc). Through incorporating coumarin groups into the hydrogels, the crosslinking degree of hydrogels could be increased by photo-crosslinking of polymer chains based on the photodimerization of coumarin groups. After the hydrogel was irradiated by a photomask under UV light (365 nm), the irradiated and unirradiated region in the hydrogel showed different crosslinking degrees, leading to different volume phase transition temperature (VPTT) in the two region of the hydrogel. The pattern in the hydrogel appeared only within a specific temperature range, and the temperature of the environment can be monitored by the prepared hydrogel sensor. After soaking the patterned hydrogel in the acidic solution, no pattern information was displayed at all temperatures, and the pattern information can only emerge by dual decryption (base and temperature). In addition, the information can be erased by UV light (254 nm), which further ensures information security. This work provide a new way for low-cost unpowered temperature sensors and information encryption with more security.
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Nano Energy
·
2023
·
IF 17.6
Yapeng Sun,Jiankai Zhang,Bo Yu,Shengwei Shi,Huangzhong Yu
The under-coordinated bonds and deep-level defects on the perovskite surface always act as non-radiative recombination centers and lead to energy loss . The usual surface modification efficiency is limited because of the diversity of surface terminals and defects. Here, a co-modification strategy is proposed for more-thorough modification by reconstructing and post-modifying perovskite surface defects . In detail, the tetrahydrofuran (THF) is firstly implemented to remove the organic component and expose the perovskite surface with uniform Pb terminals and defects, and then the 4-Methylbenzyl Mercaptan (MBM) is used to form strong R-S-Pb bonding with them, which achieves the increase and decrease of under-coordinated Pb donor defects. Correspondingly, the surface energy level of perovskite is observed a consistent change with defects. THF/MBM co-modification changes the perovskite surface energy level from n-type toward p-type, which enhances the holes’ transport efficiency. As a result, the best power conversion efficiency (PCE) increases from 22.23% of the control device to 24.17% of the device with THF/MBM co-modification. Notably, a full-coverage and strong-bonding protective layer is formed by THF/MBM co-modification, which facilitates excellent device stability (Retains 93.7%, after 3360 h in N 2 ). This strategy shows great potential in high-performance PSCs by reconstructing defects and energy level of perovskite surface.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 11
·2725-2734
·
IF 6.569
Di Li,Yingying Xing,Changjian Zhou,Yikai Lu,Shengjie Xu,Xiangli Shi,Deli Jiang,Weidong Shi
Due to the low-carbon economy requirement in large-scale industrial applications, exploration of active, robust, resourceful, low-cost and efficient oxygen evolution reaction (OER) electrocatalysts is urgently needed. In this work, we report a Fe–N co-doped cobalt selenide nanosheet array (Fe–N–CoSe2) on nickel foam (NF) as a highly efficient OER electrocatalyst via an anion and cation co-doping strategy using a metal–organic framework (MOF) as the precursor. The nanosheet arrays grown on NF without an additional binder are not only beneficial for accelerating the charge transfer, but also for suppressing electrocatalyst shedding. Furthermore, the nanosheet structure constructed using nanograins could promote electrolyte penetration and gas diffusion and increase the active sites. More importantly, the Fe and N element doping can further provide additional active sites, regulate the electronic structure and boost the OER kinetics. In view of the abovementioned points, the as-prepared Fe–N–CoSe2 electrocatalyst exhibits outstanding OER performance and long-term durability. It affords a current density of 50 mA cm−2 at a small overpotential of 270 mV with a Tafel slope of 62.7 mV dec−1, and the Fe–N–CoSe2 electrocatalyst has only a small attenuation of 1.9% after a 100 h constant test at 100 mA cm−2 in alkaline solution, which is superior to the commercial RuO2 electrode. These results offer a potential approach for the preparation of effective and robust OER electrocatalysts as substitutes to replace the expensive commercial electrocatalysts based on element doping.
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Journal of Physical Chemistry C
·
2021
·
IF 4.126
Pengfei Yao,Jing Cao,Xue Gong,Ce Han,Mingbo Ruan,Ping Song,Weilin Xu
The development of catalysts free of platinum-group metals with a high performance for the oxygen reduction reaction (ORR) in proton exchange membrane fuel cells is a grand challenge. Herein, we report zeolitic imidazolate framework-8-based Co, N, and S tridoped carbon frameworks (Co–N–S CFs) with high ORR catalytic activity and remarkable durability in an alkaline medium. Results indicate that the high ORR performance of the Co–N–S CFs could be attributed to the unique 3D structure of carbon frames, the synergistic effect among Co, N, and S, and its high electron conductivity. It is also found that the N and S doped heteroatoms can anchor Co atoms by forming CoNx and CoSx active sites for a highly efficient ORR. The results obtained here can help in the design and understanding of the cost-effective highly active Pt-free electrocatalysts.
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JOURNAL OF THE CERAMIC SOCIETY OF JAPAN
·
2021
·Vol. 129
·期 3
·159-167
·
IF 1.224
Yonghuan HAN,Liwen YAN,Shichen XIE,Tao XU,Wei JING,Feng HOU
Nd3xY3−3xAl5O12 (Nd:YAG) powders with high uniformity were synthesized by reverse-titration co-precipitation method. The precipitation formation process and dispersion mechanism of Nd:YAG precursor in co-precipitation process were analyzed, and the influence of the preparation technology on the dispersion of powders was explored by adjusting the concentration of precipitator, alcohol-water solvent and ratio of composite dispersant. In addition, through the analysis of the precursor calcination process, combined with SEM and particle size analysis, it is shown that, under optimum processing conditions, the powders have excellent particle uniformity, narrow particle size distribution and appropriate crystal size when calcined at 1150 °C for 2 h.
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DYES AND PIGMENTS
·
2021
·
IF 4.889
Xiaofeng Sun,Hui Wang,Jinpeng Qi,Shengju Zhou,Hongguang Li
In recent years, it is heartening to witness that carbon dots (CDs), a rising star in the family of carbon nanomaterials , have displayed tremendous applications. However, the investigations toward self-assembly of CDs are still in their infancy. Tannic acid (TA) is a naturally derived polyphenolic compound with special molecular structure. Here, the co-assembly of CDs and TA in aqueous solutions has been investigated. The CDs/TA binary mixtures exhibited rich phase behavior, which went through the process of transparent phase-turbid phase-transparent phase. We focus on investigating the morphologies of the samples. As the concentration of TA increases, the aggregates evolve from the network structures to the spherical aggregates, and finally become the vesicles. Through systemic analysis of changes of zeta potential , morphologies and size distributions at varying temperature and pH, the mechanism of aggregate formation is proposed. The effect of adding TA on the fluorescence properties of CDs aqueous solutions was studied. After integration into aggregates, the potential applications of the CDs in biology and life sciences could be significantly expanded.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Chunyu Zhang,Guozhu Liu,Bo Ning,Shuairen Qian,Danning Zheng,Li Wang
The electrochemical oxygen reduction reaction (ORR) via two-electron pathway is a sustainable way of producing hydrogen peroxide. Nanostructured carbon materials are proved to be effective catalysts for 2e − ORR. Herein, a series of mesoporous carbon with tunable nitrogen species and oxygen functional groups were synthesized by varying the added amount of dopamine hydrochloride as nitrogen and oxygen source. The modified catalysts exhibited higher content of pyrrolic-N and ether C–O groups which are confirmed by a series of characterization. Raman spectra and correlation analysis revealed that the increased proportion of defect sites in carbon materials are closely related to the introduced pyrrolic-N and ether C–O groups. And the rotating ring-disk electrode (RRDE) measurement carried out in 0.1 M KOH electrolyte showed the H 2 O 2 selectivity increased with the content of defect sites. Among them, the optimized catalyst (NOC-6M) exhibited a selectivity of 95.2% and a potential of 0.71 V vs. RHE at −1 mA cm −2 . Moreover, NOC-6M possessed the high H 2 O 2 production rate of 548.8 mmol g cat −1 h −1 with faradaic efficiency of 92.4% in a two-chamber H-cell. Further mechanistic analysis revealed that the introduction of pyrrolic-N and ether C–O are likely to improve the binding energy of the defect sites toward ∗OOH intermediate, resulting in a more favorable 2e − ORR pathway for H 2 O 2 production.
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Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 21
·12807-12817
·
IF 12.732
Hao Zhang,Chaohai Wang,Wuxiang Zhang,Ming Zhang,Junwen Qi,Jieshu Qian,Xiuyun Sun,Brian Yuliarto,Jongbeom Na,Teahoon Park,Hassanien Gomaa Abdien Gomaa,Yusuf Valentino Kaneti,Jin Woo Yi,Yusuke Yamauchi,Jiansheng Li
Carbon-based electrodes play important roles in constructing efficient capacitive deionization (CDI) devices. Therefore, the rational design of carbon materials with optimized structure, composition, and morphology is crucial for further improving the CDI performance. Herein, a novel N, P co-doped eave-like hierarchical porous carbon (NP-EHPC) for CDI is reported. To prepare the NP-EHPC, the core–shell ZIF-8@AF particles are first prepared through the kinetically-controlled growth of zeolitic imidazolate framework-8 (ZIF-8) and polymerization of p-aminophenol and formaldehyde (AF), followed by subsequent pyrolysis and post-doping with phosphorus. Owing to the unique eave-like morphology, presence of abundant mesopores, and co-doping of P and N, the NP-EHPC exhibits a high desalination capacity of 24.14 mg g−1 in 500 mg L−1 NaCl solution at 1.2 V and long cycling stability of over 150 cycles. Moreover, the density functional theory (DFT) calculation results reveal that the co-doping of N and P atoms can greatly enhance the binding energies for Na and Cl atoms and lead to superior electrosorption capacity. This work provides a new insight into the design of high-performance carbon materials for the desalination of brackish water.
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Polymers
·
2021
·Vol. 13
·期 8
·1270
·
IF 4.329
Mengyuan Zhang,Zhonghua Chang,Xiaofeng Wang,Qian Li
Biodegradable and bioabsorbable polymers have drawn considerable attention because of their mechanical properties that mimic human soft tissue. Poly(l-lactide-co-ε-caprolactone) (PLCL), the copolymer of L-lactic (LA) and ε-caprolactone (CL), has been applied in many tissue engineering and regenerative medicine fields. However, both the synthesis of PLCL and the structure-activity relationship of the copolymer need to be further investigated to allow tuning of different mechanical properties. The synthesis conditions of PLCL were optimized to increase the yield and improve the copolymer properties. The synthetic process was evaluated by while varying the molar ratio of the monomers and polymerization time. The mechanical properties of the copolymer were investigated from the macroscopic and microscopic perspectives. Changes in the polymerization time and feed ratio resulted in the difference in the LA and CL content, which, in turn, caused the PLCL to exhibit different properties. The PLCL obtained with a feed ratio of 1:1 (LA:CL) and a polymerization time of 30 h has the best toughness and elasticity. The developed PLCL may have applications in dynamic mechanical environment, such as vascular tissue engineering.Keywords:poly(l-lactide-co-ε-caprolactone);synthesis;segment;toughness;elasticity
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