APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Jiarun Cheng,Chaojie Lyu,Hangren Li,Jiwen Wu,Yue Hu,Bin Han,Kaili Wu,Mirabbos Hojamberdiev,Dongsheng Geng
An original strategy was reported to manipulate ORR selectivity of N-doped hollow mesoporous carbon spheres (N-HMCS) via heteroatom (P and S) doping. Heteroatom doping can not only modulate electronic structure of N-HMCS and proportion/configuration of doped N, but also regulate ORR pathway. Specifically, rich-graphitic N sites and electron-rich C–P bond domains in N,P-HMCS act as electron donors, making *OOH more unstable and easier to desorb into H 2 O 2 . This severely distorts the sp 2 lattice of graphene, catalyzing a two-electron ORR synergistically. Conversely, a strong interaction between electron-deficient C–S bond domain and *OOH intermediate due to the introduction of highly electronegative S hinders the desorption of *OOH, leading to the breakage of the O–O bond and promoting four-electron ORR along with the rich-pyridinic N receptor site. The reaction activity and kinetics mechanism present a positive correlation with proportion of graphitic N, revealing graphitic N is the primary active site with a much faster electron transfer capacity.
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Advanced Materials Interfaces
·
2022
·Vol. 10
·期 4
·2201817
·
IF 6.389
Junfeng Zhang,Haotian Liu,Weikang Zhu,Bin Chen,Runfei Yue,Shuoyao Yin,Na Xie,Ran Li,Yan Yin
The design of the efficient, flexible air electrode for enhancing the Zn-air batteries (ZABs) performance is vital in developing a new portable rechargeable power supply. Emerging research indicates that non-precious metal materials have promising activity for oxygen reduction/evolution in alkaline conditions while constructing a high-performance and reliable electrode is still a big challenge at the present stage. In this work, a bimetal doped zeolitic imidazolate framework (ZIF) film is synthesized by fast current-driven synthesis (FCDS) on a thin carbon nanotube film (CNTF). After carbonization at 950 °C, CoFe-N-C nanofoam formed on the CNTF, resulting in binder-free, flexible electrodes. It exhibits excellent activity and stability toward oxygen reduction and evolution. The CoFe-N-C/CNTF-based liquid-state ZAB shows an output power density of 294 mW cm −2 . When applied in solid-state ZAB, the flexible battery shows high power density and excellent cycling stability.
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Polymers
·
2022
·Vol. 14
·期 23
·5135
·
IF 4.967
Xu Han,Yun Tao,Chao Xu,Yicong Deng,Zisen Meng,Zhenhao Dou,Peng Wang,Quan Feng
Hemin possesses great potential in eliminating organic pollutants due to its mild reaction condition, light-harvesting efficiency, and environmental friendliness. However, it has drawbacks such as being easy to aggregate and hard to recycle, and poor stability should be improved in practical application. Herein, the subject developed an electrospinning approach to enable the hemin particulates to be immobilized onto polyacrylonitrile (PAN) nanofibers stably. Hydrogen peroxide (H2O2) was adopted as an oxidant in the system to simulate the enzymatic catalysis of hemin in an organism. Scanning electron microscopy (SEM), Fourier transform infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS), UV-Vis diffuse reflection spectroscopy (DRS), and electron spin resonance spectroscopy (ESR) analysis was employed to discuss the morphology, structure, and mechanism of the prepared n-hemin/PAN nanocomposite membranes, and 0.02 mmol L−1of the rhodamine B (RhB) removal activity in different conditions was also verified with these membranes. The kinetic studies showed that n-hemin/PAN nanocomposite membranes maintained excellent properties both in adsorption and degradation. Around 42% RhB could be adsorbed in the dark, while 91% RhB decolorized under xenon lamp irradiation in 110 min, suggesting the catalytic performance of n-hemin/PAN was greatly driven by light irradiation. Differing from the axial coordinated hemin complexes, n-hemin/PAN would catalyze hydrogen peroxide into •OH radicals rather than •OOH and high-valent metal-oxo species. This work provides an effective way to support hemin as nanocomposite membranes, in which the molecular interaction between polymer and hemin made their light adsorption an obvious red shift.Keywords:polyacrylonitrile;hemin;photocatalysis;enzyme-like catalysis;electrospinning
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PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Wenjie Xue,Hongxia Liu,Binbin Zhao,Lixia Ge,Shuai Yang,Minghuang Qiu,Jiong Li,Wei Han,Xinqing Chen
N-ethylcarbazole (NEC) has been considered one of the most prospective liquid organic hydrogen carriers (LOHCs) for hydrogen storage. However, designing single catalyst capable of driving both hydrogenation of NEC and dehydrogenation of dodecahydro-NEC (12 H-NEC) is of a big challenge. Herein, we develop an atomic-dispersion of Rh with the Co nanoparticles (NPs) to form a Rh 1 Co structure maximizing the Rh utilization, which boosts the reversible (de)hydrogenation of NEC, and enables multiple cycles of reversible hydrogen uptake and release. Significantly, a low temperature of 90 °C is realized for the complete hydrogenation (100%), representing one of the lowest temperatures yet reported for the total hydrogenation of NEC. The remarkable catalytic performance of Rh 1 Co catalysts is the result of the optimal electronic structure between atomic-dispersion of Rh and Co NPs confirmed by structural characterizations and density functional theory (DFT) calculations, which allowed fast interfacial electron transfer to intermediates.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Linlu Shen,Pengwei Yan,Jimin Shen,Jing Kang,Yang Shen,Binyuan Wang,Shengxin Zhao,Yingxu Gong,Yabin Li,Yizhen Cheng,Shuyu Wang,Zhonglin Chen
In this study, bromide ion (Br − ) was found to accelerate the degradation of N , N -dimethylhydrazine compounds in peroxymonosulfate (PMS) oxidation and synchronously reduce their N -Nitrosodimethylamine (NDMA) formation. Hexamethylenebis (1,1-dimethylsemicarbazide) (HDMS) and daminozide (DMZ) were selected as the model compounds to clarify the mechanisms in the presence or absence of Br − for the PMS batch oxidation experiments. In the absence of Br − , the degradation of the model compounds accompanied by the formation of NDMA was induced by the electron transfer between PMS/singlet oxygen ( 1 O 2 ) and the (CH 3 ) 2 N-N- groups of the model compounds. In the presence of Br − , the generated hypobromous acid (HOBr) was verified to account for the acceleration of the reaction. The difference in NDMA formation in PMS oxidation and PMS/Br − oxidation was related to the changes in degradation paths. The electron-withdrawing substituents Br or O of PMS or HOBr substituted the N atoms of the model compounds, generating brominated or oxidation products that were hard to be further oxidized, thus decreasing NDMA formation. Moreover, the toxicity of the products in PMS/Br − oxidation was significantly lower than in alone PMS oxidation. This work provides new insight into the unique advantage of Br − during PMS oxidation.
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International Journal of Nanomedicine
·
2023
·
IF 8
Qian Yu,Chentao Shen,Xiangsheng Wang,Zhenxing Wang,Lu Liu,Jufang Zhang
Purpose We aimed to develop an antioxidant dressing material with pro-angiogenic potential that could promote wound healing. Gelatin (Gel) was selected to improve the biocompatibility of the scaffolds, while graphene oxide (GO) was added to enhance their mechanical property. The loaded N-Acetyl cysteine (NAC) was performing the effect of scavenging reactive oxygen species (ROS) at the wound site.Materials and Methods The physicochemical and mechanical properties, NAC releases, and biocompatibility of the NAC-GO-Gel scaffolds were evaluated in vitro. The regeneration capability of the scaffolds was systemically investigated in vivo using the excisional wound-splinting model in mice.Results The NAC-GO-Gel scaffold had a stronger mechanical property and sustainer NAC release ability than the single Gel scaffold, which resulted in a better capacity for cell proliferation and migration. Mice wound-splinting models revealed that the NAC-GO-Gel scaffold effectively accelerated wound healing, promoted re-epithelialization, enhanced neovascularization, and reduced scar formation.Conclusion The NAC-GO-Gel scaffold not only promotes wound healing but also reduces scar formation, showing a great potential application for the repair of skin defects.
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PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Hao Qin,Nengjie Feng,Quan Lv,Hui Wan,Guofeng Guan
Single atomic catalysts (SAC) isolated in zeolite have been reported for hydroisomerization of n-alkanes. However, it is widely found that metal species located outside zeolite crystals have beneficial effects on catalytic performance, rather than inside zeolite. Herein, we introduce cerium oxide as a binder to anchor Pt single atoms on the catalyst surface . Pt species were atomically dispersed on catalyst surface certified by AC HAADF-STEM and XAS. Pt 1 @CeO x /SAPO-11 not only shows significant activity but also effectively inhibits the selectivity of cracking or hydrogenolysis . The turnover frequency value of 0.05%Pt 1 @CeO x/ SAPO-11 reaches 9511 h −1 , 13 times higher than reported catalyst prepared with the space-confined strategy. Reaction mechanisms have been proposed to explain the different effects of platinum status and location on the reaction. Platinum single atoms located outside the catalyst crystal are speculated more favourable to this reaction. Conceptually, catalytic efficiency of this reaction can be improved by dispersing the active sites to reduce the local concentration of the product of a reversible step in an intermediate reaction. An appropriate loading of 0.05 wt% is needed to achieve the high efficiency of the metal and acid sites simultaneously.
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高影响因子
Materials Today Communications
·
2022
·
IF 3.662
Xian-Hui Zhang,Liang-Liang Zha,Ji-Wei Chen,Chuan-Ying Wei,Bo Wu,Jun-Wei Wang,Hong-Liang Yu,Jian-Hua Wu,Xue-Feng Yan
There are numerous challenges in the low-cost batch fabrication of high-performance absorbers. A low-cost preparation process for metal-containing acrylic resin ( 3SM-yAN , y = 6, 9 and 12) employs a one-step free radical polymerization of iron (III) chloride, sodium methacrylate, and acrylonitrile. Fe-3SM-yAN was prepared using carbonization. The carbonization of metal-containing acrylic resin was performed at 800 °C in an argon atmosphere for two hours. The broadest effective absorption bandwidth (EAB) of Fe-3SM-9AN absorbing material yielded 8.07 GHz at 2 mm with a minimum reflection loss of − 36.70 dB (11.41 GHz), and the EAB could cover 14.8 GHz (3.2–18 GHz) with a tunable absorber thickness from 1.0 to 5.0 mm. The synergistic effect of impedance matching and strong electromagnetic attenuation was found to yield excellent microwave absorption of Fe-3SM-yAN （y = 6, 9 and 12）. The magnetic porous shell-like Fe-3SM-yAN is potentially highly suitable for batch production of lightweight and efficient microwave-absorbing materials.
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高影响因子
CELLULOSE
·
2022
·Vol. 29
·期 18
·9953-9967
·
IF 6.123
Wan Jiansheng,Li Hong,Cai Xiaoyu,Yan Jun,Liao Yongping
In this study, functional coatings with N-halamine structure were formed on cotton fabrics by dopamine (DA) auto-deposition and DA/Polyethyleneimine (PEI) covalent co-deposition, respectively. SEM、UV-Vis and XPS had confirmed the deposition of DA and DA/ polydopamine (PDA) on the cotton fabrics. When the mass ratio of DA/PEI was 1:1.5, a uniform functional coating was formed. XRD had indicated that the coating and the oxidative sodium hypochlorite solution did not affect the crystal structure of cellulose. The DA/PEI co-deposited modified cotton fabric had excellent antibacterial property after chlorination, and the inactivation rate against E coli and S aureus could reach 100% with a contact time of 30 min. In vitro cell cytocompatibility studies demonstrated that the DA/PEI co-deposited modified cotton fabric has good biocompatibility. The functional coating on the cotton fabric remained stable after 50 washing cycles. The UPF values and the wrinkle recovery angle (WRA) tests showed that the DA/PEI co-deposited coating imparted great durable press and UV protective properties to the cotton fabric. The breaking strength loss rate of the modified cotton fabrics after chlorination was about 20%, which had little effect on the wearing property. Graphic abstract
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Carbon Letters
·
2022
·Vol. 33
·期 2
·409-418
·
IF 3.117
Chen Liang,Yang Lanyun,Xu Chenxi,Chen Kechun,Wang Wei,Yang Liming,Hou Zhaohui
Recently, hollow carbon spheres (HCS) have aroused great interests in the field of energy storage and conversion owing to their unique morphology, structure and other charming properties. Nevertheless, unsatisfactory electrical conductivity and relatively poor volumetric energy density caused by inevitable gaps between discrete carbon spheres greatly impede the practical application of HCS. In this work, for the first time we propose a novel dual-template strategy and successfully fabricate interconnected 3D hollow N-doped carbon network (HNCN) by a facile and scalable pyrolysis process. By systematical characterization and analysis, it can be found that HNCN is assembled by HCS and lots of mesoporous carbon. Compared to the counterparts, the obtained HNCN exhibits unique 3D interconnected architecture, larger specific surface area, hierarchical meso/macropore structure, higher structure defects, higher N doping amount and more optimized N configurations (especially for pyridinic-N and graphitic-N). As a result, these advantageous features endow HNCN with remarkably promoted electrochemical performance for supercapacitor and oxygen reduction reaction. Clearly, our proposed dual-template strategy provides a good guidance on overcoming the intrinsic shortcomings of HCS, which undoubtedly broadens their application in energy storage and conversion.
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高影响因子
ACS Applied Energy Materials
·
2023
·
IF 6.4
Wenhan Jia,Hao Wu,Yunxin Zheng,Ziyi Liu,Gaotuo Cai,Jianfeng Wen,Guanghui Hu,Tao Tang,Xinyu Li,Li Jiang,Zhiyong Wang,Ming Li,Haifu Huang
Herein, we demonstrate the enhanced pseudocapacitive performance of a MoS2-based flexible supercapacitor by the co-doping strategy of cations and anions. The MoS2 nanosheet arrays on carbon cloth are directly doped with N and Co atoms through a simple hydrothermal process. The obtained cation and anion co-modified MoS2 (N-Co-MoS2) shows improved electron transport efficiency and enhanced active sites for MoS2. According to the first-principles calculations, N-Co-MoS2 has a unique band structure and high electrical conductivity. As expected, N-Co-MoS2 shows higher capacitive performance with 5072.5 mF cm–2 and a better cycle life (retaining 100% capacitance after 10,000 cycles) than pure MoS2. Furthermore, a solid-state flexible N-Co-MoS2 supercapacitor device is fabricated to demonstrate excellent mechanical stability with a specific capacitance of 3236 mF cm–2 and a stable cycle capacitance of 75.56% after 5000 cycles. In our work, we have provided a reference for preparing MoS2-based materials with good supercapacitive performance.
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高影响因子
POLYMER
·
2022
·
IF 4.432
Junping Lv,Lin Zhu,Meng Zhang,Zexu Zhao,Shu-Wei Chen,Jinyi Wang
Actuators with controllable and reversible morphing towards environment stimuli have great potential applications in diverse fields. In spite of good progress made over the past decades, simple and efficient preparation of multi-response actuators is still a challenge. Here, we report a strategy to prepare humidity and near infrared (NIR) dual-response actuators with controllable and reversible bending or twisting deformation. The actuators were made up of two layers, one was polyvinyl butyral (PVB) layer with humidity and NIR inertness, and the other was chlorine-modified polypyrrole (PPy-Cl) doped poly(N-isopropylacrylamide-co-benzophenone) (PNIPAM-ABP) composite layer, taking advantage of the NIR photothermal conversion capability of PPy-Cl, along with the thermal-responsive PNIPAM-ABP. Upon NIR light irradiation , PPy-Cl converted light energy into heat, which subsequently induced the shrinkage of poly(N-isopropylacrylamide) (PNIPAM) chains; upon a high-humidity environment, PPy-Cl absorbed water molecular and transferred it into PNIPAM polymer , which further caused the bilayer to shrink or swell in an asymmetric manner, consequently leading to reversible bending or unbending behaviors. Interestingly, upon ultraviolet (UV) light irradiation with a grid photomask, the bilayer actuators showed bending or twist behaviors along with a special direction. The bionic flowers made from the actuators could imitate sunflower's opening and closing behaviors in response to NIR or humidity. The dual-response actuator could also imitate the lifting weight behaviors of forklifts. As an interesting example for potential utilization, a smart four-wheel vehicle was constructed using the bilayer actuator, showed excellent fast-moving performance.
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