INORGANIC CHEMISTRY COMMUNICATIONS
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2023
·
IF 3.8
Yichong Chen,Jinbing Cheng,Aihua Wang,Congbin Liu,Hailong Yan,Yang Qiu,Zhongzheng Wang,Paul K. Chu,Yongsong Luo
Electrospinning is carried out to fabricate Ti 3 C 2 T x @Co nanocomposite films composed of 2D Ti 3 C 2 -encapsulated Co nanoparticles derived from Co-MOF precursors. The unique 1D nanochain structure inherits not only the high electrochemical activity, but also excellent electron and ionic conductivity. The Co nanoparticles with good conductivity and MXene with high electrochemical activity improve the electrochemical properties giving rise to high capacity and good cycling stability. The Ti 3 C 2 flakes partially accommodate the volume changes during Li + insertion/extraction and the electrospinning technique prevents self-aggregation of Ti 3 C 2 flakes and aggregation of ZIF-67 nanoparticles, consequently producing a larger surface area and more active sites on the flexible anode. As a result, the MXene/Co composite has excellent properties such as a high reversible capacity of 422 mA h g −1 after 500 charging-discharging cycles at a current density of 1 A/g and retained capacity of 177 mA h g −1 at a rate of 5 A/g. The materials and strategy have large potential in commercial energy storage devices.
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PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
·
2023
·Vol. 120
·期 48
·e2314362120
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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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Journal of Physical Chemistry C
·
2023
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IF 3.7
Li Fu,Zerui Liu,Pengjie Dong,Yingshu Guo
Screening a novel electrochemiluminescence (ECL) system and reducing electrochemical interference by lowering the ECL potential are crucial to ECL evolution. Herein, an ECL system is explored with different hydrazine compounds as coreactants and ternary CuInS2/ZnS nanocrystals (CIS/ZnS NCs) as a luminophore, demonstrating that hydrazine compounds with varied structures would assuredly affect the ECL triggering potential and efficiency. Electro-oxidized hydrazine-based coreactants containing a symmetrical structure and −N–N single bonds with strong reducibility could produce an efficient electron transfer recombination path with electro-oxidized CIS/ZnS NCs, which eventually generate efficient and low-triggering-potential ECL performance; otherwise, the hydrazine compounds with a double bond, such as −C═N or −C═O, or strong electronegative atoms would reduce the ECL efficiency and increase the ECL triggering potential, which result from double bonds or strong electronegative atoms of hydrazine compounds hindering the protonation of coreactants and then delaying the electron–hole recombination process. The structure of hydrazine-based coreactants with a −C═S double bond would competitively bond with the Cu element within CIS/ZnS NCs, contributing to the blank ECL with CIS/ZnS NCs as the luminophore. Furthermore, CIS/ZnS NCs exhibit two additional low hole injected processes under alkaline conditions through exploration of the differential pulse voltammetry (DPV) nature from CIS/ZnS NCs. The ultralow-triggering-potential of CIS/ZnS NCs around 0.11 V could be achieved by adjusting the hole injection processes of NCs and selecting pasoniazide as the coreactant, which is extremely below any previously reported ECL system. This work contributes to a deeper understanding of the ECL mechanism.
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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Wenyu Lu,Hongzhen Cai,Wenbin Zhang,Zhiqiang Qi,Keyan Yang,Xiangsheng Han
Nanoscale biochar is a promising material for the remediation of polluted water due to its low-cost sustainability, nevertheless, which still hindered by the self-aggregation and vulnerability issues in actual wastewater. In this work, biochar nanosheets (BCN) were successfully molded into membranes and aerogels with the help of aramid nanofibers (ANF) through a co-assembled process. Ascribing to the improved molecular sieving effects and electrostatic interactions of co-assembled membranes, as well as the superior chemical and thermal stabilities, the resultant ANF/BCN x membranes exhibited favorable dye separation performances toward rhodamine 6 G (R6G) even under high-temperature (e.g., ∼96.1 L·m −2 ·h −1 ·bar −1 and ∼97.4% at 80 °C) and strong acidic conditions (e.g., ∼84.1 L·m −2 ·h −1 ·bar −1 and ∼97.9% for 10 wt% H 2 SO 4 solutions). Besides, due to the reduced vaporization enthalpy, the ANF/BCN x aerogels as solar steam generators also demonstrated promising capability for clean water production even in 5 wt% H 2 SO 4 solutions (an evaporation rate of ∼1.0 kg·m −2 ·h −1 and an impressive efficiency of ∼89.9% under one sun illumination). Compared to conventional biochar materials, this work offered simple feasible morphology engineering designs to prepare multifunctional biochar-based composites with unique co-assemble structures, while also demonstrated great potential in wastewater remediation under extreme conditions.
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ENERGY & FUELS
·
2023
·
IF 5.3
Chuanhong Wang,Xuefang Chen,Shimiao Yao,Fen Peng,Lian Xiong,Haijun Guo,Hairong Zhang,Xinde Chen
The morphology and regeneration ability of adsorbents are important for gas pressure swing adsorption and separation. Herein, HCP-1 (a hyper-crosslinked polymer) and HCP@MAO(Fe) (a hyper-crosslinked polymer modified by ferrocene) with a spherical morphology are synthesized by a post-crosslinking reaction of chloromethylated styrene-divinylbenzene (Cl-St-DVB) beads for the separation of CO2/CO and CO2/CH4. Both static adsorption and dynamic separation tests verified that HCP@MAO(Fe) has the best gas adsorption and separation performance. The highest adsorption capacity of CO2 reached 1.24 mmol/g. The IAST selectivity of CO2/CO is up to 20.6. Moreover, HCP@MAO(Fe) can be regenerated by simple vacuum operation, contributing to the low value of adsorption enthalpy (24.5 KJ/mol). The adsorption mechanism between CO2 and the resin framework was also studied by experiments and electrostatic potential map analysis. A stronger interaction can be found between CO2 and HCP@MAO(Fe) as a result of the higher Mulliken charge of the cyclopentadiene structure.
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SYNTHETIC METALS
·
2023
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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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INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Qiong Wu,Zhuoyu Wang,Baozheng Zhao,Ruiyang Zhao,Shitao Yu,Lang Huang
Promoted ethylene glycol (EG) yield from cellulose hydrogenolysis is achieved via using Nickel-tungsten doped carbon catalysts prepared from glucose ( x %Ni- y %WO x -GC T ). Synchronously metal loading and carbon formation endow the catalyst excellent catalytic performance and high stability. Mechanistic investigations of the effects of metal loading and BrØnsted acid on EG yield are conducted. Increasing W loading promotes the content of polymerized WO x and consequently increases the amount of polytungstate species, thus lead to an improved BrØnsted acid content. Results reveal that promotion of B/L acid facilitates cellulose hydrolysis and suppresses isomerization of glucose to fructose. Besides, high W loading is beneficial for reduction of WO x to form W 5+ , producing oxygen vacancies to promote retro aldol condensation (RAC) of glucose to form acetaldehyde alcohol (an important intermediate for EG). By adopting the optimized 9%Ni-12%WO x -GC 700 catalyst, a 100% cellulose conversion with a high EG yield of 65% is obtained due to the synergistic interactions between BrØnsted acid, W 5+ and Ni 0+ active sites.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 46
·21289-21296
·
IF 3.3
Xiaodie Huang,Ziye Liu,Jingjing Tu,Changchun Ji,Ying-Hua Zhou
Hydrogen storage in chemicals is regarded as one of the sustainable techniques for tackling the energy-related challenges. However, hydrogen production from ammonia borane (NH3BH3, AB) is restricted by the inherent activity of metallic catalysts, which may be boosted by light irradiation. Herein, Pd-doped Co nanoparticles (NPs) were incorporated into a Zr-MOF composite composed of MXene-derived Ti3C2 nanosheets and UiO-66-NH2 (denoted as TUNS) by a double-solvent approach, obtaining a CoPd@TUNS composite. The optimized Co30Pd@TUNS composite exhibited outstanding catalytic activity for the complete dehydrogenation of AB within 0.6 min under 300 W Xe lamp light, with a high turnover frequency of 130.37 molH2 (molmetal)−1 min−1 at 298 K. The activity of Co30Pd@TUNS increased 10-fold under light irradiation as compared to that in the dark. For photocatalytic dehydrogenation, Co30Pd@TUNS was more active than Co30Pd@UiO-66-NH2 and Co30Pd/Ti3C2. Its excellent performance might be attributed to multiple factors including the photo-harvesting MOF generating electron–hole pairs, Ti3C2 nanosheets promoting the charge separation, and the Schottky effect facilitating electron migration to metal NPs for activating the substrate via an electron-deficient BH3 moiety, along with the attack of photogenerated hydroxyl radicals and water molecules. Moreover, the kinetic study manifested that AB dehydrogenation is a zero-order reaction with regard to the substrate. The great stability and recyclability of Co30Pd@TUNS was also confirmed after 5 runs. This study would widen a pathway for the design of an efficient MOF-based catalyst for hydrogen generation in the energy-related field.
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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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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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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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CARBOHYDRATE POLYMERS
·
2017
·
IF 4.811
Xinyu Hu,Yongmei Wang,Liangliang Zhang,Man Xu,Wei Dong,Jianfa Zhang
Salecan is a novel water-soluble extracellular β-glucan and has excellent physicochemical and biological properties. A series of hydrogels were fabricated from Salecan and poly(2-acrylamido-2-methylpropanesulfonic acid- co - N -hydroxymethyl acrylamide) (poly(AMPS- co -HMAA), PAH) by semi-IPN technique. The introduction of Salecan into the PAH network endows the system with enhanced cell adhesion properties. These semi-IPN hydrogels with open interconnected pores had pH and salt-sensitive swelling behavior. The increase in the content of hydrophilic Salecan could enhance the water uptake of the hydrogels. Rheological results indicated that the incorporation of PAH into hydrogels increased the storage modulus. The degradation property of the hydrogels can be tuned by modulating the content of Salecan and BAAm. Cytotoxicity results revealed that the hydrogels were non-toxic to COS-7 cells. All these results suggested that Salecan/PAH semi-IPN hydrogels exhibited great potential for applications in soft tissue engineering.
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