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Coatings · 2023 ·Vol. 13 ·期 6 ·1097 · IF 3.4

Heterogeneous Fenton-like Catalyzation of Nanoscale Schwertmannite for Sulfamethoxazole Degradation

Xiaoqing Meng,Lin Wang,Ying Yang,Yuqi Song,Cansheng Yuan

Sulfamethoxazole (SMX) contamination in large quantities of wastewater can cause potential environmental problems. Due to difficulty in degrading SMX by natural processes, it is necessary to develop a novel technology to solve this problem. Advanced oxidation processes (AOPs) have been identified as methods with a high potential to treat recalcitrant organic pollutants. The nanoscale schwertmannite (nano-SWT) was prepared with an indoor-temperature synthesis method facilitated by polyvinylpyrrolidone (PVP). In this study, we performed a reaction of the nano-SWT materials with Fenton-like catalysts for SMX degradation in hydrogen peroxide (H2O2) media. The findings showed that the nano-SWT prepared by addition of 0.1 g·L−1PVP (nano-SWT-n,n= 0.1) could degrade 92.5% of the SMX within 90 min at indoor temperature, which was due to the nano-SWT providing abundant reaction sites at the solid/solution interfaces. Additionally, SMX could be highly mineralized with 75% TOC removal and H2O2was efficiently utilized during the nano-SWT/H2O2process. In addition, after six cycles of Fenton-like degradation, the nano-SWT remained stable and reusable as a Fenton-like catalyst for SMX degradation. The nano-SWT performed well as a catalyst for SMX degradation. Additionally, this work provides a feasible environmental purification approach for the efficient degradation of SMX through the use of nanoscale schwertmannite as a catalyst in heterogeneous Fenton-like systems.Keywords:Fenton-like;sulfamethoxazole;nanoscale schwertmannite;degradation

CAS / MDL: 723-46-6
研究领域: 环境科学 · 化学工程 · 材料科学
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Nanomaterials · 2023 ·Vol. 13 ·期 13 ·1941 · IF 5.3

Binary Ni-Co-Based Layered Double Hydroxide Nanoneedle Arrays for High Performance of Oxygen Evolution Reaction

Zhi Lu,Zhihao Zhou,Shilin Li,Gongliang Tan,Hangtian Chen,Zishuo Ge,Chong Chen,Guangxin Wang

Low-cost and high-performance electrocatalysts are crucial for water-splitting reactions. Some non-precious metal electrocatalysts are proved to be good replacements for noble metal due to the unique electronic structure features and excellent performance. In this work, binary Ni-Co-based layered double hydroxide nanoneedle arrays electrocatalysts are synthesized on Ni foam (NF) via a hydrothermal process. The microstructure and the catalytic performance of the catalyst changes significantly by regulating the molar ratio of Ni/Co. The theoretical analysis confirmed that the as-prepared NiCo-LDH nanoneedle arrays reveal a potential behavior in oxygen evolution reaction (OER) at a lower overpotential of 305 mV at 10.0 mA cm−2and a Tafel slope of 110.38 mV dec−1. The double-layer capacitance (Cdl) is 776 mF cm−2, which indicates that there are many active sites that are exposed on the surface for the electrocatalytic reaction. The results provide an obvious reference value to other types of LDH catalysts for the development of water electrolysis.Keywords:nanoneedle;Ni-Co based;electrolysis;OER;electrocatalyst

研究领域: 材料科学 · 电化学
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ENERGY & FUELS · 2022 · IF 4.654

Se-Doped CoP Nanoneedle Arrays Grown on Carbon Cloth for an Efficient Hydrogen Evolution Reaction

Baoshu Li,Jiping Li,Xixue Liu,Jinxue Guo,Yanfang Sun,Xiao Zhang

Exploring highly active catalysts with low-price materials is urgently needed for water-splitting electrolysis. Herein, selenium-doped CoP nanoneedles construct the grass-like structure, and the nanoneedles are vertically anchored on carbon cloth (Se–CoP/CC). Scanning electron microscopy and transmission electron microscopy reveal the nanoneedle array architecture of S–CoP, which is convenient for the adsorption of molecules on active centers. The small diameter of nanoneedles is beneficial for rapid charge transfer. X-ray photoelectron spectroscopy shows the electronic structure regulation of Se incorporation, which is beneficial for the optimized catalysis activity. Electrochemical tests show that Se dopants result in more catalysis sites and faster kinetics. Endowed with these advantages, good catalytic performance of the prepared sample for hydrogen evolution is disclosed, with low overpotentials of 47 mV at 10 mA cm–2 and 145 mV at 100 mA cm–2 in alkaline solution. This work highlights a promising way to improve the performance of transition-metal-based catalysts with non-metal-doping engineering toward water electrolysis application.

研究领域: 材料科学 · 电化学
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ACS Applied Materials & Interfaces · 2019 · IF 8.456

Integrin αvβ3 Receptor Overexpressing on Tumor-Targeted Positive MRI-Guided Chemotherapy

Renuka Khatik,Zhengyun Wang,Debo Zhi,Sonia Kiran,Pankaj Dwivedi,Gaolin Liang,Bensheng Qiu,Qing Yang

Multifunctional nanomaterials with targeted imaging and chemotherapy have high demand with great challenge. Herein, we rationally aimed to design multifunctional drug delivery systems by RGD-modified chitosan (CH)-coated nanoneedles (NDs) of gadolinium arsenate (RGD-CH-Gd-AsNDs). These NDs have multifunctionality for imaging and targeted therapy. NDs on intravenous administration demonstrated significant accumulation of As ions/species in tumor tissues, which was monitored by the change in T1-weighted magnetic resonance (MR) imaging. Moreover, NDs were well opsonized in cells with high specificity, subsequently inducing apoptosis to the HepG2 cells. Consequent to this, the in vivo results demonstrated biosafety, enhanced tumor targeting, and tumor regression in a subcutaneously transplanted xenograft model in nude mice. These RGD-CH-Gd-AsNDs have great potential, and we anticipate that they could serve as a novel platform for real-time T1-weighted MR diagnosis and chemotherapy.

研究领域: 医学影像学 · 药物递送系统 · 肿瘤学
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ACS Applied Materials & Interfaces · 2022 · IF 10.383

RuO2-Incorporated Co3O4 Nanoneedles Grown on Carbon Cloth as Binder-Free Integrated Cathodes for Tuning Favorable Li2O2 Formation

Xiaohui Peng,Mingzhe Li,Lihua Huang,Qizhe Chen,Weiwei Fang,Yuyang Hou,Yusong Zhu,Jilei Ye,Lili Liu,Yuping Wu

Developing ideal Li–O2 batteries (LOBs) requires the discharge product to have a large quantity, have large contact area with the cathode, and not passivate the porous surface after discharge, which put forward high requirement for the design of cathodes. Herein, combining the rational structural design and high activity catalyst selection, minor amounts of RuO2-incorporated Co3O4 nanoneedles grown on carbon cloth are successfully synthesized as binder-free integrated cathodes for LOBs. With this unique design, plenty of electron–ion–oxygen tri-phase reaction interface is created, the side reaction from carbon is isolated, and oxygen reduction reaction/oxygen evolution reaction (OER) kinetics are significantly facilitated. Upon discharge, film-like Li2O2 is observed growing on the needle surface first and eventually ball-like Li2O2 particles form at each tip of the needle. The cathode surface remains porous after discharge, which is beneficial to the OER and is rare in the previous reports. The battery exhibits a high specific discharge capacity (7.64 mAh cm–2) and a long lifespan (500 h at 0.1 mA cm–2). Even with a high current of 0.3 mA cm–2, the battery achieves a cycling life of 200 h. In addition, punch-type LOBs are fabricated and successfully operated, suggesting that the cathode material can be utilized in ultralight, flexible electronic devices.

CAS / MDL: 10026-22-9 57-13-6
研究领域: 材料科学 · 电化学
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GREEN CHEMISTRY · 2024 · IF 9.3

Trace F-doped Co3O4 nanoneedles for enhanced acidic water oxidation activity via promoting OH coverage

Genyan Hao,Tao Zhao,Qiang Fang,Yunzhen Jia,Dandan Li,Dazhong Zhong,Jinping Li,Qiang Zhao

Exploring Earth-abundant and efficient electrocatalysts to replace Ir and Ru for the acidic oxygen evolution reaction (OER) is essential to reduce the cost of clean hydrogen production. Here, we show that trace amounts of electronegative non-metallic element fluorine (F)-doped Co3O4 nanoneedles improve the activity and stability of Co3O4. The F-doped Co3O4 nanoneedles supported on carbon paper (F-Co3O4/CP) exhibit an overpotential of 350 mV at 10 mA cm−2 for the acidic OER. In addition, their performance remains consistent after continuous operation for 80 h. Detailed investigations reveal that introducing an anion promotes the enrichment of OH on the surface of Co3O4 and prevents acid corrosion, thereby enhancing the intrinsic OER activity and stability. Theoretical calculations further indicate that F doping can effectively improve electron transfer and optimize the energy barrier for the formation of *OOH intermediates, which significantly improves OER performance. This study provides guidance for designing efficient and stable non-noble metal acidic water oxidation catalysts.

CAS / MDL: 10026-22-9 57-13-6
研究领域: 材料科学 · 电化学
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CHEMISTRY-A EUROPEAN JOURNAL · 2019 ·Vol. 26 ·期 18 ·4120-4127 · IF 5.16

Interfacial Engineering FeOOH/CoO Nanoneedle Array for Efficient Overall Water Splitting Driven by Solar Energy

Chunyu Qiu,Suqi He,Yuan Wang,Qingxiang Wang,Chuan Zhao

Graphical Soak up the sun : A vertically aligned FeOOH/CoO nanoneedle array with a clear synergistic interface for solar energy-driven water splitting was engineered by a simple impregnation method. Interface engineering has been applied as an effective strategy to boost the electrocatalytic performance because of the strong coupling and synergistic effects between individual components. Here, we engineered vertically aligned FeOOH/CoO nanoneedle array with a synergistic interface between FeOOH and CoO on Ni foam (NF) by a simple impregnation method. The synthesized FeOOH/CoO exhibits outstanding electrocatalytic activity and stability for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in an alkaline medium. For the overall water splitting, the bifunctional FeOOH/CoO nanoneedle catalyst requires only a cell voltage of 1.58 V to achieve a current density of 10 mA cm −2 , which is much lower than that required for IrO 2 //Pt/C (1.68 V). The FeOOH/CoO catalyst has been successfully applied for solar cell-driven water electrolysis, revealing its great potential for commercial hydrogen production and solar energy storage.

研究领域: 材料科学 · 能源科学
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CHEMICAL ENGINEERING JOURNAL · 2022 · IF 16.744

Hierarchical heterostructure of NiFe2O4 nanoflakes grown on the tip of NiCo2O4 nanoneedles with enhanced interfacial polarization effect to achieve highly efficient electrocatalytic oxygen evolution

Xingzhao Wang,Jiabing Luo,Yongxiao Tuo,Yufeng Gu,Wanli Liu,Shutao Wang,Yan Zhou,Jun Zhang

In this work, a heterostructure oxygen evolution reaction (OER) electrocatalyst consisting of NiFe 2 O 4 nanoflakes grown on the tip of NiCo 2 O 4 nanoneedles arrays supported on nickel foam (NCO-NNs@NFO-NFs/NF) was obtained via simultaneous cation (Co 3+ by Fe 3+ ) and ligand exchange (-OH by 1,4-benzenedicarboxylic acid) and further annealing of the hydroxide/MOF precursor in air. HRTEM and Raman characterizations confirm the formation of NCO/NFO heterostructure. XPS characterization and charge density difference calculations clarify the electron transfer from Fe to Ni and Co at the NCO/NFO heterointerface. Electrochemical tests show that NCO-NNs@NFO-NFs/NF possesses excellent OER electrocatalytic activity (overpotential of 265 mV@50 mA cm −2 ) and durability (stable for 100 h@1 A cm −2 ). NCO-NNs@NFO-NFs/NF‖20 % Pt/C two-electrode system can achieve 10 mA cm −2 at 1.398 V for anion exchange membrane (AEM) water splitting in 1.0 M KOH at 85 °C, which exceeds the activity of using commercial RuO 2 as an anode at 25 °C, combined with the stability of 100 h at 10 mA cm −2 at 25 °C, demonstrating the practical application in industrial AEM process. XPS and HRTEM characterizations of NCO-NNs@NFO-NFs/NF after the OER V - t test, along with ex-situ Raman characterization, confirm that Co and Fe sites undergo surface reconstruction to form specific CoOOH/FeOOH interfaces, as to exert the synergistic effect of Co and Fe dual active sites during OER process. DOS calculations reveal that the density of state at Fermi energy level increases after the introduction of Fe, thereby improving conductivity and facilitating the activation of adsorbed oxygen species. This study shows a significant methodology for simultaneous improvement of the electrocatalytic stability and activity of spinel oxides-based heterostructures, which is critical for practical application.

CAS / MDL: 10025-77-1
研究领域: 材料科学 · 电化学 · 能源转换
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

Unravelling the enhanced capacitive desalination behavior of nanoneedle-like NiFe2O4

Gengen Peng,Zehao Zhang,Haibo Li

In this work, the nanoneedle-like NiFe 2 O 4 (NFO) has been prepared by a template method and post annealing process for capacitive deionization (CDI) with enhanced performance. Owing to the unique structure, the nanoneedle-like NFO provides large accessible surface area, which benefits to offer abundant electroactive sites for electrosorption. Meanwhile, the salty ions diffusion and electron exchange are promoted by needle-like structure. Further, it is found that the NFO annealed at 450 °C (NFO-450) demonstrate the high crystallinity, rich mesopores and exceptional electrochemical properties. As electrode for CDI, the NFO-450 has manifested the high desalting capacity of 1.62 mmol/g when the effective loading mass of both electrodes is 23.6 mg. Interestingly, the desalting capacity realizes the linear correlation with the mass of NFO electrode ranging from 23.6 to 45.8 mg. The mechanism analysis stands out that the Na + are captured by NFO, accompanied by the reduction of Ni 3+ to Ni 2+ in the 1 st cycle. Afterwards, the Na + can be electrostatically removed by the NFO//AC system.

研究领域: 材料科学 · 环境工程
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POLYMER · 2025 · IF 4.5

A simple superhydrophilic/underwater superoleophobic PVDF-OH/AA@ZnO membrane with needle structures for efficient oil-in-water emulsions separation

Zhanjian Liu,Ping Wang,Jing Jing,Meiling Li,Yuxin Fu,Xiguang Zhang,Huaiyuan Wang

Superwetting oil-water separation membranes are effective materials for treatment of wastewater containing emulsified oil, but the problem of membrane pollution remains a huge challenge during its long-term operation. In this study, we successfully developed a superhydrophilic/underwater superoleophobic membrane using a simple phase separation method. The fabrication process involved three key steps: (1) surface hydroxylation of pristine PVDF using NaOH etching to generate active hydrogen bonds and hydroxyl groups, (2) acrylic acid (AA) grafting onto the hydroxylated PVDF surface to introduce carboxyl functionalities, and (3) in-situ chelation of needle-like ZnO onto the AA-grafted matrix. The synergistic effect of the surface needle-like ZnO and the hydration layer endowed the PVDF-OH/AA@ZnO membrane with an outstanding oil-water separation efficiency of n-hexane up to 99.68 %, and higher than 98 % for various emulsions (e.g. kerosene, petroleum ether, chloroform, and dichloromethane) under gravity. Moreover, compared with the basement membrane, the tensile strength of the modified membrane increased from 106.21 kPa to 153.84 kPa, indicating its excellent mechanical properties under strong external forces. The PVDF-OH/AA@ZnO membrane demonstrated exceptional recycling performance, with a separation efficiency above 97.25 % after five cycles, and exhibited anti-fouling capability with simple water rinsing used to remove surface oil residues. Overall, this study provides a scalable strategy for the design of superhydrophilic/underwater superoleophobic separation membranes for the practical treatment of oily wastewater.

研究领域: 材料科学 · 环境工程
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Interfacial coupling of Ce-CoSe2 nanoneedle arrays with MXene for efficient overall water splitting

Ao Zhou,Wenwen Cai,Weijian Guo,Jizhen Ma,Yueqing Wang,Jintao Zhang

Designing highly effective, low-cost bifunctional electrocatalysts without noble metals for overall water splitting remains a significant challenge. In this work, interfacial coupling of Ce-doped CoSe 2 nanoneedle arrays with MXene (Ce-CoSe 2 /MXene) is developed via the facile hydrothermal and selenization methods. The extensive specific surface area and favorable hydrophilicity of Ti 3 AlC 2 , combined with the optimized electronic structure and abundant active sites from Ce-doping and selenization, contribute to the exceptional bifunctional electrocatalytic performance of the Ce-CoSe 2 /MXene electrode. Specifically, this heterostructure achieves a low hydrogen evolution reaction (HER) overpotential of 34 mV at 10 mA cm −2 , an oxygen evolution reaction (OER) overpotential of 279 mV at 100 mA cm −2 , and an overall water splitting (OWS) potential as low as 1.45 V at 10 mA cm −2 . In-situ Raman spectroscopy reveals that surface reconstruction would improve catalytic activity and stability. Theoretical calculations indicate that the Ce-CoSe 2 /MXene can improve the adsorption of intermediates and facilitate HER/OER process by lowering the kinetic barrier, thereby enhancing electrocatalytic activity. This research marks a substantial advancement in the development of low-cost, efficient electrocatalysts for overall water splitting.

研究领域: 材料科学 · 电化学
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APPLIED SURFACE SCIENCE · 2021 · IF 6.707

Straw-like phosphorus-doped Co2MnO4 nanoneedle arrays supported on nickel foam for high-efficiency hydrogen evolution reaction in wide pH range of electrolytes

Ru-Lan Zhang,Jiu-Ju Feng,You-Qiang Yao,Ke-Ming Fang,Lu Zhang,Zheng-Zhi Yin,Ai-Jun Wang

Developing high-performance and cut-price non-noble-metal electrocatalysts for hydrogen evolution reaction (HER) is desirable yet challenging. Herein, straw-like phosphorus-doped Co 2 MnO 4 nanoneedle arrays supported on nickel foam (P-Co 2 MnO 4 /NF) were prepared by successive hydrothermal treatment, oxidation and P doping for high-efficiency HER. Benefiting from the unique needle-like arrays and compositions advantages, P-Co 2 MnO 4 /NF exhibited excellent HER activities with the overpotentials of 33, 43 and 102 mV to afford a current density of 10 mA cm −2 in alkaline, acidic and neutral media, respectively, coupled with the long-term electrochemical stability. This work affords an effective avenue for preparation of cost-effectiveness, high-efficiency and wide-pH HER catalysts for electrochemical energy technologies.

研究领域: 材料科学 · 电化学
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