JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Guoqiang Liu,Yuwen Cheng,Maoqin Qiu,Chengcheng Li,Anyang Bao,Zhongti Sun,Cuizhen Yang,Dongming Liu
Designing high-activity electrocatalysts to enhance the slow multielectron-transfer process of the oxygen evolution reaction (OER) is of great importance for hydrogen generation. Here, we employ hydrothermal and subsequent heat-treatment strategies to acquire nanoarrays-structured NiO/NiCo 2 O 4 heterojunction anchored Ni foam (NiO/NiCo 2 O 4 /NF) as efficient materials for catalyzing the OER in an alkaline electrolyte. Density functional theory (DFT) results demonstrate that NiO/NiCo 2 O 4 /NF exhibits a smaller overpotential than those of single NiO/NF and NiCo 2 O 4 /NF owing to interface-triggered numerous interface charge transfer. Moreover, the superior metallic characteristics of NiO/NiCo 2 O 4 /NF further enhance its electrochemical activity toward OER. Specifically, NiO/NiCo 2 O 4 /NF delivered a current density of 50 mA cm −2 at an overpotential of 336 mV with a Tafel slope of 93.2 mV dec −1 for the OER, which are comparable with those of commercial RuO 2 (310 mV and 68.8 mV dec −1 ). Further, an overall water splitting system is preliminarily constructed via using a Pt net as cathode and NiO/NiCo 2 O 4 /NF as anode. The water electrolysis cell performs an operating voltage of 1.670 V at 20 mA cm −2 , which outperform the Pt net||IrO 2 couple assembled two-electrode electrolyzer (1.725 V at 20 mA cm −2 ). This study proposes an efficient route to acquire multicomponent catalysts with rich interfaces for water electrolysis.
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高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 14
·4389-4397
·
IF 4
Yujun Wu,Wei Shuang,Lin Yang,Chuanbao Cao
Graphene-based materials have been regarded recently as a promising substance for electrochemical energy conversion and storage devices owing to their unique structure and extraordinary properties. Herein, an enormously facile one-step pyrolysis approach is reported for the fabrication of ternary (P,S,N)-doped graphene, which is further investigated as an efficient metal-free electrocatalyst for the oxygen reduction reaction (ORR). Furthermore, optimized ternary-doped graphene can deliver excellent ORR catalytic activity that favors the four-electron ORR process and outstanding long-term durability (90.54% current retention after 20000 s which is far superior to that of commercial Pt/C) owing to the preferable synergetic coupling effect between P, S and N. Density functional theory (DFT) calculations were performed to reveal the synergetic coupling effect between doping elements in the ORR process. This work provides an extremely simple one-step pyrolysis method for the synthesis of P,S,N-doped graphene for electrochemical energy conversion and storage devices.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Handong Jiao,Mengjun Liu,Zhe Wang,Manpeng Lin,Zhaoliang Qu,Jianxun Song,Shuqiang Jiao
Molten salt electrorefining is expected to be a powerful technology for upcycling titanium scrap because of its robust ability of removing impurities. However, realizing the stable operation of electrorefining, for example, the current efficiency of the anode and the cathode is still a key challenge from the viewpoint of industrial applications. Here, we study titanium’s anodic dissolution and cathodic deposition processes via a direct three-dimensional visualization method based on a computed tomography technology under high-temperature operational conditions. Real-time quantitative results show that the current efficiency is obviously affected by the concentration of titanium ions in the melt. Visual analysis of the local dissolution rate and the curvature of the titanium anode at different electrolysis stages reveals the kinetic origin of the concentration-induced current efficiency changes, which arise from the priority of the side reactions being dependent on the concentration of titanium ions. Finally, we show that employing the high concentration and single existence forms of titanium ions is an effective strategy to prevent the side reactions and improve the current efficiency. This work provides a fresh and fundamental understanding of the side reactions occurring at the interface of electrodes and is significant for facilitating the stability of electrorefining engineering of titanium.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Wen-Chao Geng,Jing-Jing Li,Ji-Long Sang,Yu-Xin Xia,Yong-Jun Li
Pt-based multi-metallic electrocatalysts containing hetero-junctions are found to have superior catalytic performance to composition-equivalent counterparts. However, in bulk solution, controllable preparation of Pt-based hetero-junction electrocatalyst is an extremely random work owing to the complexity of solution reactions. Herein, we develop an interface-confined transformation strategy, subtly achieving Au/PtTe hetero-junction-abundant nanostructures by employing interfacial Te nanowires as sacrificing templates. By controlling the reaction conditions, composition-varied Au/PtTe can be easily obtained, such as Au 75 /Pt 20 Te 5 , Au 55 /Pt 34 Te 11 , and Au 5 /Pt 69 Te 26 . Moreover, each Au/PtTe hetero-junction nanostructure appears to be an array consisting of side-by-side Au/PtTe nanotrough units and can be directly used as a catalyst layer without further post-treatment. All Au/PtTe hetero-junction nanostructures show better catalytic activity towards ethanol electrooxidation than commercial Pt/C because of the combining contributions of Au/Pt hetero-junctions and the collective effects of multi-metallic elements, where Au 75 /Pt 20 Te 5 exhibits the best electrocatalytic performance among three Au/PtTe nanostructures owing to its optimal composition. This study may provide technically feasible guidance for further maximizing the catalytic activity of Pt-based hybrid catalysts.
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高影响因子
Energy Technology
·
2023
·Vol. 11
·期 8
·2300118
·
IF 3.8
Peiyao Pan,Qingle Zeng,Xiaoxiao Li,Chao Liu,Jinming Zeng,Tongxiang Liang,Xiaopeng Qi
Electrocatalytic water splitting provides an effective way to store electrical energy (i.e., solar and wind energy) intermittently. It is believed that developing electrocatalysts with excellent stability, high catalytic efficiency, and abundant natural reserves is the key to the industrialization of electrochemical water splitting. Herein, nickel–molybdenum electrocatalyst formed on the surface of a low-cost etched stainless-steel mesh via a one-step electrodeposition method exhibits a low hydrogen evolution overpotential of 53 mV and oxygen evolution overpotential of 261 mV at a current density of 10 mA cm −2 due to the synergistic effect of nickel and molybdenum. Moreover, the as-prepared catalyst demonstrates superior hydrogen evolution reaction (HER) catalytic performance than commercial Pt/C at current density exceed 200 mA cm −2 . The electrocatalyst also shows excellent HER and oxygen evolution reaction stabilities at high current density attribute to the tightly bond between electrocatalyst and the etched stainless-steel mesh, as well as the surface reconstruction of catalyst during the cycle test. The facile electrodeposition method has lower requirements on production equipment, using stainless steel mesh as the basement reduces the production cost, the nickel–molybdenum alloy possesses excellent electrolytic water splitting performance and stability. These results indicate that this work can provide an idea for the industrialization of electrochemical water splitting.
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Small
·
2023
·Vol. 19
·期 34
·2301640
·
IF 13.3
Fan Zhang,Renjie Ji,Xiaoyang Zhu,Hongke Li,Yating Wang,Jingpeng Wang,Fei Wang,Hongbo Lan
Highly active bifunctional electrocatalysts for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) have always been the key factors to affect the performance of zinc–air batteries. However, integrating the independent reaction sites of ORR and OER in a catalyst remains a major challenge. Herein, a collaborative strategy based on defect induction and doping is proposed to prepare the strain-regulated Pt–NiO@Ni sub-micron particles (Pt–NiO@Ni SP). Benefiting from the synergistic effect of tensile strain and Pt-doped, the metallic Ni-based sub-micron particles with tensile strain as the catalyst carriers can effectively optimize the electronic distribution of atomic structures in Pt and NiO on the surface of particles, leading to reduce the energy barrier of intermediates for ORR and OER. Consequently, the Pt–NiO@Ni SP exhibits outstanding bifunctional catalytic activity with the ΔE index of 0.65 V under a low Pt loading, outperforming that of the benchmark Pt/C+IrO 2 catalysts (0.76 V). Impressively, the Pt–NiO@Ni SP-based liquid zinc–air battery develops a high open-circuit potential (1.47 V), excellent energy density (188.2 mW cm −2 ), and favorable cyclic charge–discharge cycling durability (200 h at 20 mA cm −2 ). This work provides an innovative avenue for the rational construction of highly active bifunctional electrocatalysts for practical applications.
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JOURNAL OF PHARMACEUTICAL SCIENCES
·
2023
·
IF 3.8
Wenxuan Cao,Jingbao Chen,Long Wu,Yu hang Xu,Yun Meng,Xiang Li,Zhiyun Zheng,Xiaoqin Chu
Purpose The aim of this study was to develop liquid crystal (LC) precursors to obtain novel long-acting analgesics for injection based on depot systems and compare the difference between the cubic and hexagonal precursors in delivering Diclofenac sodium (DS). Methods Diclofenac sodium liquid crystal precursor injections were prepared and characterized, followed by in vitro release, pharmacodynamic , and pharmacokinetic studies. Results The optimal formulations were prepared with a ratio of Phytantriol/ethanol/water as 76:19:5 for cubic LC precursors, and a ratio of Phytantriol/ethanol/water/Vitamine-E acetate as 72:18:5:5 for hexagonal, both loading various drug dosages (2.5%, 3.75% and 5%), respectively. Polarized light microscopy and small angle diffraction confirmed that the precursors were isotropic fluids and transformed into gels with Pn3m or HII framework in water. Rheological studies have shown that precursors belong to Newtonian fluids and gels to pseudoplastic fluids. The release showed that the DS in the commercial injection (DS-inj) was completely liberated within 6 h, whereas only 46.55% and 49.73% of the DS in 2.5% cubic precursors and 2.5% hexagonal precursors were freed, respectively. Pharmacodynamic studies have shown that cubic, hexagonal and DS-inj raised the pain threshold in mice by 169.4%, 157.3% and 113.79%, respectively. The mean retention times of DS in cubic and hexagonal were 3.16 and 2.67 times longer than DS-inj, respectively, according to pharmacokinetic results. Conclusion In conclusion, cubic and hexagonal are both promising analgesic sustained release formulations. In addition, based only on the current comparison, cubic seems to have a better long-acting effect.
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Advanced Energy Materials
·
2023
·Vol. 13
·期 22
·2300325
·
IF 27.8
Zhen Zhang,Tianping Wang,Weiwen Wang,Xiangnan Wang,Xianglin Luo,Chong Cheng,Xikui Liu
Metallophthalocyanines (MPcs) hold great promise in the electrochemical reduction of oxygen; however, their practical applications in energy storage and conversion are still limited by their low stability and poor water oxidation activity. Herein, a novel stable 2D imide-linked metalphthalocyanine framework (denoted as FePc-PI) is reported, that has atomically dispersed Fe-N 4 sites deposited on the KB substrate via in situ growth, followed by incorporation of ultrafine nickel oxide nanoparticles (NiO x @FePc-PI/KB) to induce bifunctional electrocatalytic activities for the oxygen reduction reaction and oxygen evolution reaction. Benefitting from the robust aromatic backbone, the engineered catalytic centers, and the unique electronic structures owing to the interaction between the Fe-N 4 sites and NiO x species, the newly developed NiO x @FePc-PI/KB catalyst exhibits excellent reversible oxygen bifunctional activity ( E 1/2 = 0.926 V, η 10 = 285 mV), delivering a record-low overpotential difference (Δ E ) of 0.59 V, which far exceeds the noble-metal-based Pt/C+RuO 2 benchmark (Δ E = 0.77 V) and represents the highest level for reported bifunctional electrocatalysts. Furthermore, the rechargeable aqueous Zn-air batteries assembled with the NiO x @FePc-PI/KB catalyst deliver a high peak power density of 232.9 mW cm −2 and long-term cycling durability over 1400 cycles. Flexible all-solid-state Zn-air batteries exhibit stable cycling at various flat/bent/flat states, thus demonstrating their excellent prospects in realistic implementations.
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Advanced Healthcare Materials
·
2023
·
IF 10
Tianyi Zheng,Yanyun Pang,Daixing Zhang,Yue Wang,Xu Zhang,Huijie Leng,Yingjie Yu,Xiaoping Yang,Qing Cai
Natural bone tissue possesses inherent electrophysiological characteristics, displaying conductivity and piezoelectricity simultaneously; hence, the reconstruction of local electrical microenvironment at defect site provides an effective strategy to enhance osteogenesis. Herein, a composite cryogel-type scaffold (referred to as Gel-PD-CMBT) is developed for bone regeneration, utilizing gelatin (Gel) in combination with a conductive poly(ethylene dioxythiophene)/polystyrene sulfonate matrix and Ca/Mn co-doped barium titanate (CMBT) nanofibers as the piezoelectric filler. The incorporation of these components results in the formation of an integrated piezoelectric/conductive network within the scaffold, facilitating charge migration and yielding a conductivity of 0.59 S cm −1 . This conductive scaffold creates a promising electroactive microenvironment, which is capable of up-regulating biological responses. Furthermore, the interconnected porous structure of the Gel-PD-CMBT scaffold not only provides mechanical stability but also offered ample space for cellular and tissue ingrowth. This Gel-PD-CMBT scaffold demonstrates a greater capacity to promote cellular osteogenic differentiation in vitro and neo-bone formation in vivo. In summary, the Gel-PD-CMBT scaffold, with its integrated piezoelectricity and conductivity, effectively restores the local electroactive microenvironment, offering an ideal platform for the regeneration of electrophysiological bone tissue.
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高影响因子
IONICS
·
2023
·Vol. 29
·期 7
·2853-2864
·
IF 2.8
Wang Wenping,Zhao Zhiyi,Deng Jiayao,Lang Wei,Zhen Lipeng,Lu Huimin
The oxygen reduction reaction of the cathode in an Al-air battery plays a key role in the performance of the entire battery. Generally, Pt and its alloys are recognized as catalysts with high oxygen reduction catalytic performance, but their application is limited by the rare earth content and high cost. In this paper, α-MnO 2 nanotubes are prepared using a hydrothermal method and used as a template. Nano-Ni–Mn bimetallic oxides with different compositions are prepared with different NiO and α-MnO 2 ratios by calcination. The effects of morphology, phase, and Mn 3+ /Mn 4+ and Ni 3+ /Ni 2+ ratios on electrochemical performance and battery discharge performance are analyzed. The results show that the contents of α-MnO 2 and Ni 6 MnO 8 in NM-12 catalyst are low, and the molar ratio of Mn 3+ /Mn 4+ and Ni 3+ /Ni 2+ is high. Also, the specific surface area of NM-12 is relatively high. Finally, the catalyst prepared with a NiO to α-MnO 2 ratio of 1:2 shows better electrochemical catalytic performance and battery discharge performance that is comparable to that obtained for a commercial 20 wt% Pt/C catalyst.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Xiang Wan,Kai Shi,Huan Li,Fangxie Shen,Shan Gao,Xiangmei Duan,Shen Zhang,Chunning Zhao,Meng Yu,Ruiting Hao,Weifang Li,Gen Wang,Maria Peressi,Yinchang Feng,Weichao Wang
Catalytic decomposition of aromatic polluters at room temperature represents a green route for air purification but is currently challenged by the difficulty of generating reactive oxygen species (ROS) on catalysts. Herein, we develop a mullite catalyst YMn2O5 (YMO) with dual active sites of Mn3+ and Mn4+ and use ozone to produce a highly reactive O* upon YMO. Such a strong oxidant species on YMO shows complete removal of benzene from −20 to >50 °C with a high COx selectivity (>90%) through the generated reactive species O* on the catalyst surface (60 000 mL g–1 h–1). Although the accumulation of water and intermediates gradually lowers the reaction rate after 8 h at 25 °C, a simple treatment by ozone purging or drying in the ambient environment regenerates the catalyst. Importantly, when the temperature increases to 50 °C, the catalytic performance remains 100% conversion without any degradation for 30 h. Experiments and theoretical calculations show that such a superior performance stems from the unique coordination environment, which ensures high generation of ROS and adsorption of aromatics. Mullite’s catalytic ozonation degradation of total volatile organic compounds (TVOC) is applied in a home-developed air cleaner, resulting in high efficiency of benzene removal. This work provides insights into the design of catalysts to decompose highly stable organic polluters.
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Inorganics
·
2023
·Vol. 11
·期 4
·170
·
IF 2.9
Zikang Lu,Rikai Liang,Yuqi Shao,Weiju Hao
Achieving high−efficiency and stable hydrogen evolution from water splitting is a great challenge. Herein, a facilely prepared two−dimenssional self−supported catalytic electrode with excellent stability is constructed for large−scale hydrogen production from alkaline simulated seawater. The bifunctional catalytic electrode is prepared by a fast and mild one−step of sodium borohydride etching on a nickel foam (NF) substrate without adding other additives (NF@NiBx−3h). The overpotential of the hydrogen/oxygen evolution reaction (HER/OER) in alkaline−simulated seawater at 10 mA cm−2is 96 mV and 261 mV. At 200 mA cm−2, the NF@NiBx−3h electrode shows good stability over 7 days throughout the water splitting process due to the corrosion resistance of the NF substrate, and strong adhesion between the Ni−B active material and the substrate. This work demonstrates a novel strategy for fabricating catalytic electrodes with high−performance, low cost and excellent stability.Keywords:mild and fast construction;chemical etching;HER;OER;industrial−grade water splitting
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危险品化学品经营许可证（带存储）