ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Junfeng Zhang,Shuo Zhao,Bin Chen,Shuoyao Yin,Yingjie Feng,Yan Yin
Anion-exchange membrane water electrolyzer (AEMWE) is attracting attention for hydrogen production owing to its ability to employ nonprecious metal catalysts and high energy conversion efficiency. Spinel-structured transition metal oxides exhibit excellent potential in oxygen evolution reaction (OERs). Nevertheless, the research on highly active and durable spinel-structured electrodes for the anodic OER of AEMWE is deficient. Herein, a self-supported S-CoCu oxide/nickel foam (S-CoCuOx/NF) anode was synthesized through a two-step method (electrodeposition and sulfidation). The formation of abundant oxygen vacancies and heterostructure collaboratively enhances the electron and mass transfer, resulting in an overpotential of 313 mV at 100 mA cm–2 for OER. For the lab-scale AEMWE system with the S-CoCuOx/NF anode, a current density of 1 A cm–2 was obtained at 1.87 V (cell voltage) with high durability for 110 h (1 A cm–2) at 60 °C. The results will provide insights into developing the spinel structure-derived anode for high-performance AEMWE.
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CORROSION SCIENCE
·
2023
·
IF 8.3
Feng-Ting Li,Zhi-Kun Wang,Yi Zhou,Li-Zhi Li,Yue-Qi Liu,Li Wang,Chun-Ling Li,Hua-Feng Zhu,Shuang-Qing Sun,Song-Qing Hu
Chemical modification is effective in improving the corrosion inhibition efficiency of carbon dots (CDs) on steel. Here, the imidazolium ionic liquids (IL) modified-CDs (IL-CDs) are synthesized and proved to be mixed-type corrosion inhibitors . The IL increases the pyrrole N content and facilitates the formation of a denser inhibitor film. Molecular simulations confirm that the IL reduces the π-π interaction between CDs, endowing IL-CDs with higher water solubility and better corrosion inhibition effect than CDs. The lower orbital energy gap and larger positive electrostatic potential distribution enable the inhibition efficiency of IL-CDs of 97.11% in 1 M HCl, much superior to CDs (90.80%).
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jia-Yi Shi,Zhen-Long Wang,Ke-An Wang,Hai-Bin Zhu
The electrochemical reduction of carbon dioxide into energy-carrying compounds or value-added chemicals is of great significance for diminishing the greenhouse effect. However, it is still imperative to replace the less-value anodic oxygen evolution reaction (OER) to improve the technical economy. Herein, we firstly reported a bifunctional CuS/TiO 2 catalyst for both anodic methanol oxidation reaction (MOR) and cathodic carbon dioxide reduction (CO 2 R). The in-built abundant CuS/TiO 2 heterointerfaces are found to boost the CO 2 R and MOR to produce formate. Based on the unique bifunctionality of CuS/TiO 2 , a paired electrosynthesis of formate was performed with a total Faradaic efficiency (FE) of about 170 %, in which the cathodic CO 2 R achieved a formate FE of about 70 %, and the anodic MOR exhibited an almost 100 % formate FE.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2023
·
IF 11.4
Xuening Wang,Zhao Jiang,Jieshu Qian,Wanyi Fu,Bingcai Pan
In the development of nanoenabled technologies for large-scale water treatment, immobilizing nanosized functional materials into the confined space of suitable substrates is one of the most effective strategies. However, the intrinsic effects of nanoconfinement on the decontamination performance of nanomaterials, particularly in terms of structural modulation, are rarely unveiled. Herein, we investigate the structure evolution and decontamination performance of iron (hydr)oxide nanoparticles, a widely used material for water treatment, when confined in track-etched (TE) membranes with channel sizes varying from 200 to 20 nm. Nanoconfinement drives phase transformation from ferrihydrite to goethite, rather than to hematite occurring in bulk systems, and the increase in the nanoconfinement degree from 200 to 20 nm leads to a significant drop in the fraction of the goethite phase within the aged products (from 41% to 0%). The nanoconfinement configuration is believed to greatly slow down the phase transformation kinetics, thereby preserving the specific adsorption of ferrihydrite toward As(V) even after 20-day aging at 343 K. This study unravels the structure evolution of confined iron hydroxide nanoparticles and provides new insights into the temporospatial effects of nanoconfinement on improving the water decontamination performance.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·
IF 19
Huijie Wang,Jiaye Zhu,Xuhui Ren,Yun Tong,Pengzuo Chen
Tuning coordination environment of single-atom catalysts (SACs) is widely applied for the electrochemical CO 2 reduction reaction (CO 2 RR). However, the influence of the interaction between SACs and support on the catalytic performance are not comprehensive. Herein, taking cobalt phthalocyanine (CoPc) as a conceptual example, a hetero S-atom doping strategy of hollow carbon sphere (S-NHC) is put forward as a carrier, revealing the intrinsic relationship between microenvironment regulation and catalytic activity of single Co-atom. The additional S doping may induce more carbon defect and increases the content of pyrrolic N in the S-NHC sample, leading to stronger electronic interaction of heterogeneous CoPc/S-NHC for boosting CO 2 RR performance. Remarkably, the catalyst achieves a highest CO selectivity of nearly 100% at −0.6 V, and the FE CO are over 90% in a wide potential range from −0.4 to −0.8 V in a flow cell. The maximum power density is high as 2.68 mW cm −2 at 4.7 mA cm −2 for the Zn–CO 2 battery with CoPc/S-NHC cathode. In situ attenuated total reflection infrared (ATR-IR) spectroscopy reveals the formation of key *COOH and *CO intermediates, while the calculation result confirm the optimized Gibbs free energy of these intermediates on CoPc/S-NHC, suggesting the feasibility of the regulation strategy.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lixiong Xu,Yifan Yang,Chenyue Li,Rongqian Ning,Jun Ma,Mengqin Yao,Shuo Geng,Fei Liu
The electrocatalytic glycerol oxidation reaction (GOR) is an efficient way to reduce the overpotential of the anodic reaction of electrocatalytic water splitting with abundant high-value byproducts. However, it has always been difficult to reveal a clear reaction path and real active site during the electrocatalytic glycerol oxidation reaction (GOR) process. In this work, NiOOH/Ni 3 S 2 /NF, a model catalyst was synthesized by the two-step method, and the reaction path of the electrocatalytic oxidation of glycerol on NiOOH/Ni 3 S 2 /NF was clearly unveiled by the in situ infrared and Raman analysis. In addition, the TEM after GOR and in-situ Raman intuitively demonstrated that the NiOOH was the real active site during the GOR process. Consequently, the synthesized NiOOH/Ni 3 S 2 /NF catalyst achieved a current density of 10 mA cm −2 at 1.227 V vs . RHE and obtained a high formic acid Faraday efficiency of 97.7 % at a low potential of 1.4 V vs . RHE. This work demonstrates an effective method for unveiling the GOR mechanism and the other relevant electrocatalytic reaction processes.
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Materials Science & Engineering C-Materials for Biological Applications
·
2020
·
IF 5.88
Lina Ding,Yi Chang,Pengfei Yang,Weihua Gao,Mengmeng Sun,Yameng Bie,Lin Yang,Xiaoming Ma,Yuming Guo
Photothermal therapy (PTT) can take advantage of the photothermal effects of photothermal agents to acquire the energy from laser irradiation and convert it into heat. This can intensively elevate the temperature of the surrounding environment to directly destroy the cancer cells. It is expected that PAs with strong absorption in near infrared (NIR) range might possess the ideal tissue-transparent feature and minimal damage to surrounding healthy tissues, beneficial to the practical application. Herein, well-dispersed L-cysteine modified MoS 2 (MoS 2 -Cys) nanospheres with the average diameter of about 422 nm and strong NIR adsorption were successfully synthesized through a facile method. The as-prepared MoS 2 -Cys nanospheres are composed of nanosheets with the average thickness of about 13.7 nm. The photothermal conversion efficiency of the as-prepared MoS 2 -Cys nanospheres with the very low concentration of 50 μg/mL was determined to be 35% when exposed to 808 NIR laser at the power density of 0.8 W/cm 2 , much higher than those of the previous reports with same dose and power density. MoS 2 -Cys nanospheres possessed the good photothermal ablation effect to significantly inhibit the growth of tumor in vivo . Furthermore, MoS 2 -Cys nanospheres did not exhibit detectable side effects, suggesting their good in vitro and in vivo biocompatibility.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Ziyong Chang,Baili He,Xiaosha Gong,Xiaoyue Qi,Kexin Liu
Preparation of efficient adsorbents is of great significance for the recovery of precious metals from secondary resources. Herein, –NH 2 was successfully grafted on MIL-101(Cr) via hydrothermal reaction to improve the adsorption capacity of Au (Ⅲ) in aqueous solution. MIL-101(Cr)–NH 2 had a huge specific surface area (1016.50 m 2 ‧g −1 ), which can provide more adsorption sites for Au (III). At 298 K, the maximum adsorption capacity of Au (III) by MIL-101(Cr)–NH 2 was 792.43 mg∙g −1 and was higher than that by MIL-101(Cr) (140.83 mg∙g −1 ). The adsorption data was well fitted by Langmuir and pseudo-second-order models, confirming that the adsorption process conformed to single molecule adsorption and chemical adsorption . Mechanism study indicated that the adsorption of Au (III) by MIL-101(Cr)–NH 2 was initiated with electrostatic attraction and promoted by reduction and inner complexation between AuCl 4 - and protonated amino groups. During adsorption, Au (Ⅲ) was reduced to Au (0) and Au (I) by –NH 2 . Density functional theory (DFT) calculation demonstrated that MIL101(Cr)–NH 2 possessed higher binding affinity and more adsorption sites for Au (III) than MIL-101(Cr). Moreover, MIL-101(Cr)–NH 2 exhibited excellent selectivity towards Au (III) and good recyclability, which is promising in the recovery of precious metals.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
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IF 5.2
Haiming Fan,Liuyang Yang,Dalei Zhang,Huiliang Wu,Yuhui Yang,Zhiyi Wei,Xiaonan Huang,Yefei Wang,Songda Liu
Environmental-friendly epoxy (EP) composite coatings are regarded as distinguished candidates for preventing metal corrosion. In this paper, we synthesized a novel GO-PDA-MoS 2 /EP nanocomposite coating system by modifying dopamine (PDA) functionalized graphene oxide (GO) with MoS 2 . Here, the effect of different MoS 2 additions on the corrosion resistant properties of coatings was investigated by altering the ratio of MoS 2 to GO-PDA via electrochemical measurements, long-duration immersion experiments, and water contact angle tests. The results indicated that 0.3 wt .% MoS 2 can substantially enhance the interfacial compatibility between EP and GO-PDA and the GO-PDA-MoS 2 -0.3 wt .%/EP coating presented optimum corrosion resistant properties. Specifically, the impedance modulus (|Z|) of the GO-PDA-MoS 2 -0.3 wt .%/EP coating still reached 2.36 × 10 7 Ω·cm 2 after 30 days immersed, which was two orders of magnitude higher than pure EP coatings. This work demonstrates a novel economical and environmental scheme that MoS 2 can be employed to enhance the corrosion resistant properties and improve the interfacial interactions of EP coatings.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 33
·11204-11212
·
IF 6.4
Zhimin Mao,Su-Yun Zhang,Duo Zhao,Xiaoliang Weng,Chenxu Kang,Hui Fang,Yu-Jia Zeng
The development of metal–organic framework (MOF) materials with multifunctionalities has boosted their prospects in the fields of spintronics and optoelectronics. However, incorporating magnetic and optoelectronic properties in MOF materials remains challenging. Herein, the in situ synthesis of Cu-MOF-74, a typical one-dimensional linear magnet, is systematically investigated, which shows ferromagnetic and antiferromagnetic interactions along the axial chain direction, and overall tilted antiferromagnetism at low temperatures. In particular, the introduction of SnS:Co quantum dots (QDs) enhances the antiferromagnetic coupling, which increases the phase transition temperature of the MOF from 7.8 K to 275 K at 1000 Oe. In addition, it is demonstrated that Cu-MOF-74 possesses both magnetic and optoelectronic properties. It is found that the responsivity and detectivity of the Cu-MOF-74 photodetector are both significantly improved by the SnS:Co QDs. This research provides promising methods for concurrent improvement of the magnetic and optoelectronic properties of MOF materials, advancing in-depth research on the MOF film as a new type of semiconductor for spintronic and optoelectronic devices.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Shiyue Hu,Junhong Liu,Xuanlan Luo,Qiqi Shen,Yu Qin,Haikun Hu,Jinhai Yuan,Shuangkou Chen,Di Xu
Currently, photocatalytic degradation is a fascinating technology due to its capability to treat escalating environmental problems by degrading chemicals like dyes and pharmaceuticals from wastewater. Herein, the hexagonal prism GQDs/h-MoO 3 composite photocatalyst was fabricated through a facile hydrothermal approach. The synthesized samples were identified by XRD , SEM, FT-IR, XPS , UV-Vis DRS , and PL technologies to study the crystal structure, morphology, surface chemical composition , and optical properties . The preparation circumstances of binary compounds, such as different GQDs (Graphene quantum dots) loading amounts, precursor solution pH, hydrothermal temperature, and hydrothermal time were optimized, also, and the photocatalytic activity of materials is determined by photodegradation of Methylene Blue in this approach, which systematically investigated the impact of operational conditions on the efficiency of the photocatalytic reaction. The results revealed that 10GQDs/h-MoO 3 has the best photocatalytic performance among competitors, which exhibited a high photodegradation efficiency (85.58%) of MB, and the rate was approximately 2.13 times greater than pristine h-MoO 3 . Moreover, the PL and EIS measurements proved the outstanding separation and migration ability of the photo-excited carriers of composite, which was attributable to the fact that GQDs can serve as electron transporters and acceptors to induce electron-hole separation efficiently. Finally, the free radical scavenging experiments confirmed that the primary active species was h + in the photocatalytic process, as well as a potential explanation for the improved photocatalytic activity of GQDs/h-MoO 3 photocatalysts was proposed.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Junyuan Zhang,Ziwei Deng,Shuli Bai,Changyu Liu,Mengchen Zhang,Chao Peng,Xiaolong Xu,Jianbo Jia,Tiangang Luan
In this work, potassium acetate (KAc) was added during the synthesis of a Zn-Fe based metal-organic framework (Fe-ZIF-8) to increase the fixed amount of Fe while simultaneously enhancing the number of pores. Electrospinning was utilized to embed KAc-modified Fe-ZIF-8 (Fe-ZIF-8-Ac) into the polyacrylonitrile nanofiber mesh, to obtain a network composite (Fe@NC-Ac) with hierarchical porous structure. Fe@NC-Ac was co-pyrolyzed with thiourea , resulting in Fe, N, S co-doped carbon electrocatalyst . The electrochemical tests indicated that the prepared catalyst displayed relatively remarkable oxygen reduction reaction (ORR) catalytic activity, with an onset potential (E onset ) of 1.08 V (vs. reversible hydrogen electrode, RHE) and a half-wave potential (E 1/2 ) of 0.94 V, both higher than those of the commercial Pt/C (E onset = 0.95 V and E 1/2 = 0.84 V), respectively. Assembled into Zn-air batteries, the optimized catalyst exhibited higher open circuit voltage (1.698 V) and peak power density (90 mW cm −2 ) than those of the commercial 20 wt% Pt/C (1.402 V and 80 mW cm −2 ), respectively. This work provided a straightforward manufacturing strategy for the design of hierarchical porous carbon-based ORR catalysts with desirable performance.
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