JOURNAL OF BIOMATERIALS SCIENCE-POLYMER EDITION
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2023
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IF 3.6
Meng-qiu Xia,Jingbao Chen,Liu Liu,Chun-ling Tian,Wang-kai Cheng,Zhiyun Zheng,Xiao-qin Chu
Primary dysmenorrhea is a common disease in women, and oral administration of Ibuprofen (IBU) is associated with first-pass effects and gastrointestinal irritation. Here, we developed ibuprofen-loaded hexagonal liquid crystal (IBU HLC) gel for transdermal administration. In this study, the structure of prepared IBU HLC was characterized using polarizing microscopey (PLM) and small angle X ray diffraction (SAXS). In vitro drug release behavior and percutaneous penetration were investigated, and drug transdermal behavior was observed by confocal laser scanning microscope (CLSM). Finally, the pharmacokinetic profile and tissue distribution were investigated after transdermal administration. The PLM and SAXS results showed that the inner structure of IBU HLC was hexagonal phase. Moreover, in vitro release, skin permeation and CLSM demonstrated that IBU HLC had an excellent sustained-release effect, and a good transdermal penetration effect accompanied by the combination of multiple percutaneous routes. Pharmacokinetic studies indicated that IBU entered the blood circulation through abdominal transdermal administration in small amounts, mainly entering the uterus, and had a certain targeting ability. In conclusion, the IBU HLC gel would be a promising sustained-release preparation for transdermal administration to relieve dysmenorrhea with a significant drug concentration in the uterus.
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ELECTROCHIMICA ACTA
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2023
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IF 6.6
Weiwei Han,Fan Zhang,Yi He,Chunlin Yu,Lecheng Lei,Xingwang Zhang
Developing highly efficient noble-metal-free bifunctional nanocatalysts for electrocatalytic water splitting is attractive but challenging. Notably, the rational structure engineering could effectively promote electronic transfer and improve the active area. Herein, a free-standing N-doped porous carbon nanosheet arrays encapsulated with metallic Co nanoparticles electrocatalyst (Co@NC-A) for overall water splitting was designed via pyrolysis process followed with acid treatment. The N-doped carbon matrix not only enhances electron mobility and protects the metallic Co nanoparticles from electrolyte corrosion, but also improves the electrochemically active area and facilitates mass transfer. Consequently, the Co@NC-A exhibits superior electrocatalytic performance toward OER ( η 10 = 270 mV) and HER ( η 10 = 162 mV) in 1 M KOH. Moreover, the Co@NC-A as a bifunctional catalyst in overall water splitting could approach 10 mA cm −2 at a cell voltage of 1.66 V and operate stably for 50 h. Combined with the density functional theory (DFT) calculations, the improvement of the HER and OER activities is also attributed to the modified electronic structure with N-doped carbon and the optimized free energy toward the adsorption/desorption of intermediates. This work provides a novel and facile non-precious metal catalyst for water splitting and should be instructive for designing more carbon-based nanocatalysts.
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ACS Sustainable Chemistry & Engineering
·
2023
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IF 8.4
Jianjun Zhu,Xinyu Zheng,Yikai Lu,Huamei Tong,Mengyue Qi,Yu Liu,Di Li,Deli Jiang
The construction of multicomponent coupled interfaces is crucial to designing highly effective and robust bifunctional electrocatalysts for water splitting. Transition metal sulfides are widely applied as efficient catalysts, but building strong coupling interfaces to enhance electrocatalytic properties remains a tremendous challenge. Here, we reported a distinctive heterostructure electrocatalyst consisting of conductive polypyrrole (PPy)-decorated cobalt–molybdenum sulfide (CoS2/MoS2) nanosheets supported on nickel foam (CoS2/MoS2@PPy/NF) using a simple two-step hydrothermal and subsequent electrodeposition approach. Experimental results reveal that the interfacial coupling and synergistic effect between the conductive PPy and CoS2/MoS2 with tunable electronic configuration are favorable for the charge transport and the electronic structure optimization of the coupled interface, where this integrated PPy can improve the conductivity and offer a guarantee for the durability of CoS2/MoS2@PPy/NF. Density functional theory (DFT) calculations verify that electronic interaction and charge redistribution in heterogeneous CoS2/MoS2 can flexibly adjust the interfacial electronic configuration and lower the d-band center. Thanks to the advantages mentioned above, the obtained CoS2/MoS2@PPy/NF exhibits outstanding catalytic properties with the overpotentials of 46 mV for the hydrogen evolution reaction (HER) and 231 mV for the oxygen evolution reaction (OER) at 10 mA cm–2. Remarkably, assembled CoS2/MoS2@PPy/NF || CoS2/MoS2@PPy/NF only acquires 1.52 V at 10 mA cm–2 in 1.0 M KOH with a durability of 50 h. This study affords a significant reference for designing bimetallic sulfide/polymer catalysts toward high-efficiency overall water splitting.
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Nano Research
·
2023
·Vol. 16
·期 8
·10881-10889
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IF 9.9
Wei Xueer,Cheng Jiawei,Li Yubing,Cheng Kang,Sun Fanfei,Zhang Qinghong,Wang Ye
The noble metal-based bimetallic clusters with high atom utilization and surface energy have been widely applied in heterogeneous catalysis, but the stabilization of these metastable clusters in harsh reaction conditions is quite challenging. Herein, we synthesize a series of Pt-, Pd-, and Ru-based clusters promoted by a second non-noble metal (Zn, Cu, Sn, and Fe), which are confined inside silicalite-1 (pure silica, S-1) crystals by a ligand-protected method. The second metal could well stabilize and disperse the noble atoms inside the rigid S-1 zeolites via Si-O-M bonds, thus enabling to lower the usage of expensive noble metals in catalysts. The as-synthesized bimetallic catalysts exhibited excellent performance in non-oxidative propane dehydrogenation (PDH) reaction, which is typically operated above 500 °C. The PtZn@S-1, PtCu@S-1, and PtSn@S-1 with only a ∼ 0.17 wt.% Pt loading offer a significant enhancement in PDH performance compared with the conventional PtSn/Al 2 O 3 catalyst with a 0.5 wt.% Pt loading prepared by impregnation method. Notably, the PtSn@S-1 provides a propane conversion of 45% with a 99% propylene selectivity at 550 °C, close to the thermodynamic equilibrium. Furthermore, the PtSn@S-1 exhibits excellent stability during 300 h on stream and high tolerance to regeneration by a simple calcination step.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
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IF 22.1
Xinyu Chen,Chuntao Chen,Majeed Muhammad Amjad,Dongping Sun,Bianjing Sun,Kai Zhang
Ruthenium (Ru)-based electrocatalysts are regarded as promising for applications in hydrogen evolution reactions (HER) due to their suitable metal-hydrogen (M-H) bonding energy. However, the strong affinity for adsorbed hydroxyl groups (OH ad ) leads to the inactivation of Ru active sites, leading to unsatisfactory performance in practical HER applications. Herein, a competitive adsorption strategy for the design of crystalline lattice-confined atomic Ru in Tungsten Carbide Nanoislands is reported. Benefiting from the unique "island–multi-atoms" structural features, Ru/WC x exhibits ultra-high mass activity (6000 mA mg −1 ) and excellent turnover frequency (3.89 H 2 −1 ) at − 100 mV vs. RHE, which is 9.5 and 51.2 times higher than commercial 20% Pt/C, respectively. In-depth mechanistic analysis demonstrates that the strength of Ru-OH ad is regulated by the oxophilicity of W atoms and the stronger W-OH ad bond to alleviate Ru site inactivation, thus enhancing the HER activity. This strategy provides a novel concept for designing advanced catalysts.
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Small
·
2023
·Vol. 19
·期 48
·2304258
·
IF 13.3
Weiju Hao,Rikai Liang,Shiheng Liang,Bonan Liu,Yunlong Qian,Ding-Kun Ji,Guisheng Li
How to mildly structure a high intrinsic activity and stable catalytic electrode to realize long-term catalytic water splitting to produce hydrogen at a wide range of pH values at industrial high current is a challenge. Herein, this work creatively proposes to prepare industrial-grade catalytic electrodes with high efficiency and stability at high current density through carbon quantum dots (CDs) modification nickel sulfide on hydrophilic flexible filter paper via one-step mild chemical plating (denoted as CDs-Ni 3 S 2 @HFP). The intrinsic activity and surface area, electron transfer ability, and corrosion resistance of Ni 3 S 2 material are increased due to the regulation, homogenous, and high concentration doping of CDs. The overpotential of the flexible catalytic electrode is only 30, 35, and 87 mV in 1 m KOH, simulated seawater (1 m KOH + 0.5 m NaCl), and neutral electrolyte (0.5 m PBS) at a current density of 10 mA cm −2 . More attractively, the CDs-Ni 3 S 2 @HFP electrode achieves over 500 h of efficient and stable catalysis at industrial high current density (500 mA cm −2 ). Due to the advantages of mild, universal, and large-area preparation of catalytic materials, this work provides technical support for flexible catalytic electrodes in efficient catalysis toward water splitting, energy storage, and device preparation.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Xinyu Chen,Diwei Shi,Min Bi,Jiexi Song,Yanqing Qin,Shiyu Du,Bianjing Sun,Chuntao Chen,Dongping Sun
Ensuring the consumption rate of noble metals while guaranteeing satisfactory hydrogen evolution reaction (HER) performance at different pH values is imperative to the development of Ru-based catalysts. Herein, we design a Mott-Schottky electrocatalyst (Ru/CeO 2 ) with a built-in electric field (BEF) based on density functional theory (DFT). The Ru/CeO 2 achieves the criterion current density of 10 mA cm −2 at overpotentials of 55 mV, 80 mV, and 120 mV in alkaline, acidic and neutral media, respectively. Both theoretical calculations and experimental analysis confirm that the improved HER activity in the Ru/CeO 2 catalyst could be due to the successful construction of BEF at the interface between the prepared Ru clusters and CeO 2 . Under the action of BEF, the electron-deficient Ru atoms can optimize the adsorption energy of H* and H 2 O and thus promote HER kinetics. Furthermore, the Ru/CeO 2 catalyst delivers a power density of approximately 94.5 mW cm −2 in alkaline-acidic Zn-H 2 O cell applications while maintaining good H 2 production stability. In this work, we optimize the electrocatalytic performance of the Ru/CeO 2 catalyst through examination of the interfacial BEF electrical charge, which combines hydrogen production with power generation and provides a promising method for sustainable energy conversion.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Xiaoqi Zhao,Yingxiao Li,Xue Zhang,Yanfang Gao,Ling Liu
Surface oxygen vacancy increases active site numbers, and multidimensional cross-linked structure improves the exposure of active sites. Thereby, they can enhance the oxygen reduction reaction (ORR) performance of Fe-N-C catalysts effectively. Herein, Fe(NO 3 ) 3 ·9H 2 O and carbon nanotubes (CNTs) were introduced into zeolitic imidazolate framework nano leaves (ZIF-L) to prepare multidimensional cross-linked Fe-N-CNTs with surface oxygen vacancies through co-pyrolysis at the high-temperature. As expected, the synthesized multidimensional cross-linked Fe-N-CNTs-900-0.2 composite rich in oxygen vacancies increased the conduction band potential and improved the reducing capacity. Thus, Fe-N-CNTs-900-0.2 possessed a better ORR electrochemical performance (half-wave potential = 0.892 V vs. RHE) that surpass the Pt/C catalysts. Moreover, the Al-air batteries containing Fe-N-CNTs-900-0.2 displayed a higher maximum power density than those of Pt/C catalysts. The electronic band structure shows that Fe-N-CNTs-900-0.2 rich in oxygen vacancy concentration has higher conduction band potential and effectively improves the activity of ORR catalysts. This work innovatively proposes that the joint work of multidimensional cross-linked structure and oxygen defects is an effective method to enhance the ORR performance and clarifies its internal reaction mechanism, which provides a new idea to design and preparer Fe-N-C catalysts.
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ChemSusChem
·
2023
·
IF 8.4
Jing Bai,Hao Li,Yuting Zhu,Yiping Zhu,Chenguang Wang,Haiyong Wang,Yuhe Liao
Graphical From the hardwood : A route was developed to transform hardwood lignin toward 2,6-dimethoxy- p -aminophenol with high yield and keeping the inherent functional groups. Lignin was first oxidized to syringaldehyde, which was converted toward 2,6-dimethoxy- p -aminophenol via oxidation, oximation, and hydrogenation. The presence of the methoxy group guaranteed the high selectivity. Although the multiple functional groups in biomass offer notable chances for producing high-value chemicals, most of the current studies focused on the (deep) defunctionalization of biomass and its derivates. Herein, we present a catalytic approach to valorize birch wood lignin with maintaining the methoxy and hydroxy groups in the final product (i. e., 2,6-dimethoxy- p -aminophenol), which has applications in different sectors such as pharmaceuticals. The proved approach involves four steps with a high yield (19.8 wt % on the basis of used lignin) to 2,6-dimethoxy- p -aminophenol. The native lignin in birch wood was first converted using alkaline aerobic oxidation in the presence of copper ions toward high-yield syringaldehyde, which was then selectively oxidized toward 2,6-dimethoxy-1,4-benzoquinone using H 2 O 2 and V 2 O 5 . Oximation of 2,6-dimethoxy-1,4-benzoquinone can selectively form 2,6-dimethoxy-1,4-benzoquinone-4-oxime, which can be quantitatively hydrogenated toward 2,6-dimethoxy- p -aminophenol. This work highlights the unique potential of biomass and its derivates for the sustainable production of high-value products with exploring the value of inherent functional groups.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Mian Li,Fei Guo,Lan Xiao,Yibin Wang,Yingjie Zhang,Xiangjie Bo,Tingting Liu
Designing two-dimensional (2D) porous carbon nanosheets is a promising strategy for enhancing the water-splitting activities of non-noble metal catalysts . In this study, we developed a novel method for synthesizing the novel three-dimensional (3D) hierarchically porous iron–nickel (FeNi) nanoparticles encapsulated in boron (B) and nitrogen (N)-codoped porous carbon nanosheets (denoted as FeNi@BNPCNS). Owing to the advantages of morphology and structure of B and N, 10.31 atom % of B/N active centers were successfully doped into the optimal FeNi@BNPCNS-800 nanosheets . FeNi@BNPCNS-800 exhibited better hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) electrocatalytic activities than control catalysts in an alkaline solution. However, the HER and OER electrocatalytic activities of FeNi@BNPCNS-800 were slightly lower than 20 wt% Pt/C and RuO 2 . The FeNi@BNPCNS-800||FeNi@BNPCNS-800 electrolyzer achieved 10 mA cm −2 at 1.514 V, which was 73 mV lower than that of 20 wt% Pt/C||RuO 2 electrolyzer (1.587 V). The perfect 3D honeycomb-like architectures, abundant mesopores/defects, and abundant electrocatalytic active sites were attributed to the outstanding water-splitting performances of FeNi@BNPCNS-800 nanosheets . This study provides an efficient strategy for the large-scale, rapid, and low-cost fabrication of 2D porous carbon nanosheets without using any template, surfactant , or expensive raw material, thus presenting a simple approach to design advanced non-noble metal electrocatalysts for water splitting.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yun Wu,Rui Yao,Kaiyang Zhang,Qiang Zhao,Jinping Li,Guang Liu
The use of proton exchange membrane (PEM) hydrolysis technology holds promise for eco-friendly hydrogen production using renewable energy sources. However, developing efficient, cost-effective, and durable bifunctional electrocatalysts for the acidic oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) remains challenging. Here, we synthesized RuO 2 /CeO 2 heterojunction loaded on carbon spheres (RuO 2 /CeO 2 @C) via hydrothermal and annealing techniques to address this issue. Our experiments demonstrate exceptional catalytic activity of RuO 2 /CeO 2 @C for both OER and HER, with overpotentials of 170 and 120 mV, respectively, at 10 mA/cm 2 in 0.5 M H 2 SO 4 . Moreover, the electrocatalyst enables overall water splitting at 1.54 V and maintains stability for over 100 h at 10 mA/cm 2 . Density functional theory (DFT) calculations suggest that RuO 2 /CeO 2 heterojunction modifies d-band center of Ru, balances H adsorption/desorption behavior, accelerates reaction kinetics, and lowers the energy barrier, thereby enhancing electrocatalytic activity. These findings provide valuable insights for future efficient bifunctional water splitting electrocatalyst design.
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iScience
·
2023
·
IF 5.8
Qing Zhang,Chen Fang,Yanlan Wang,Xiang Liu
Summary In the winter months, the temperature in most of the Earth stays below 0°C; the average temperature in winter at the South Pole is about −60°C. Therefore, it is urgent to develop efficient catalytic systems for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis at subzero temperatures. For solving the freezing issue of water at below 0°C, herein, we have employed a facile and surfactant-free approach to synthesize M-Pt/C nanocomposites (M = Pd, Rh, Ru, Ni, Cu, or Fe), by the alloying of commercial Pt/C with Pd, Rh, Ru, Cu, Ni, or Fe for selective and efficient H 2 evolution upon NH 3 BH 3 hydrolysis in saline solution at below 0°C, even at −15°C. In addition, NH 3 BH 3 hydrolysis over Pd-Pt/C in the saturated NaCl solution is utilized not only for safe hydrogen production but also for its in situ hydrogenation reduction in organic chemistry, which could avoid using dangerous hydrogen cylinders.
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