Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 19
·4274-4286
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IF 7
Jingge Zhang,Enna Ha,Danyang Li,Shuqing He,Luyang Wang,Shaolong Kuang,Junqing Hu
Nanozymes mediated catalytic therapy can produce toxic reactive oxygen species (ROS) and destroy the metabolic balance of tumor cells, providing a new direction for cancer treatment. However, the catalytic efficiency of a single nanozyme is limited by the complexity of the tumor microenvironment (hypoxia, GSH overexpression, etc.). In order to overcome these problems, we designed flower-like Co-doped FeSe2 (Co–FeSe2) nanozymes by a simple wet chemistry method. Co–FeSe2 nanozymes not only exhibit high POD and OXD-mimicking activities for facile kinetics, but also effectively consume over-expressed glutathione (GSH), inhibiting the consumption of generated ROS and destroying the metabolic balance of the tumor microenvironment. These catalytic reactions trigger cell death through apoptosis and ferroptosis dual pathways. More importantly, under the NIR II laser irradiation, the catalytic activities of Co–FeSe2 nanozymes are boosted, confirming the photothermal and catalytic synergistic tumor therapy. This study takes advantage of self-cascading engineering that offers new ideas for designing efficient redox nanozymes and promoting their clinical translation.
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Advanced Energy Materials
·
2021
·Vol. 12
·期 1
·2102359
·
IF 29.368
Yuan Chang,Panlong Zhai,Jungang Hou,Jijun Zhao,Junfeng Gao
Faced with grave climate change and enormous energy demands, effective catalysts have become more and more important due to their significant effects on reducing fossil fuels consumption. The hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) by water splitting are feasible ways to produce clean sustainable energy. Here, atomic structures and related scanning tunneling microscope images of Se defects in PtSe 2 are systematically explored. The equilibrium fractions of vacancies under variable conditions are predicted in detail. In addition, it is found that the vacancies are highly kinetically stable, without recovering or aggregation. The Se vacancies in PtSe 2 can dramatically enhance the HER performance, comparing to Pt(111). It is also revealed that a PtSe 2 monolayer with Se vacancies is also a good OER catalyst. The excellent bipolar catalysis of Se vacancies is further confirmed by experimental measurements. A defective PtSe 2 made via direct selenization of Pt foil at 773 K using a chemical vapor deposition process is produced. It is shown that the HER and OER performance of defective PtSe 2 is much more efficient than Pt foils by a series of measurements. This work, with its compelling theoretical and experimental studies indicates PtSe 2 with Se defects is an ideal bipolar candidate for HER and OER.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Yuhang Han,Jie Yuan,Yuhang Zhu,Qiangqiang Wang,Lin Li,Maosheng Cao
Microwave absorption materials can protect humanity from harmful electromagnetic radiation , but it is still a challenge to absorb electromagnetic radiation with different bands simultaneously. Herein, an effective strategy for obtaining WSe 2 @CNTs nanohybrids is reported. The conductive network and polarization of WSe 2 @CNTs nanohybrids can be tailored by confinedly implanting WSe 2 nanosheets on multi-walled carbon nanotubes. The electromagnetic properties and microwave absorption performance of the nanohybrids are effectively adjusted via changing the hybrid ratio of WSe 2 and CNTs . Multi-band microwave absorption is achieved with up to three bands. The reflection loss (RL) of the sample can reach −60.1 dB, and the bandwidth can reach 4.24 GHz (RL ≤ −10 dB). The excellent microwave absorption performance is attributed to the conductance and multiple relaxations, as well as the synergistic effect of the two. This result confirms that WSe 2 @CNTs nanohybrids are potential candidates for high-efficiency microwave absorbers and provide a valuable pathway for designing high-performance microwave absorption materials in the future.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Lei Tan,Jiangtao Yu,Haiyan Wang,Hongtao Gao,Xien Liu,Lei Wang,Xilin She,Tianrong Zhan
NiSe 2 /Ni 3 Se 4 dual-phase electrocatalysts are synthesized by calcining the Ni(OH) 2 nanosheets on Ni foam and Se powder under an N 2 atmosphere. The Ni’s charge-state, phase compositions, and electrocatalytic performances are dependent on the initial mass ratios of Ni to Se. The experimental results demonstrate that the electrocatalyst with a higher Ni charge-state and more Ni 3 Se 4 phase facilitates oxygen evolution reaction (OER), whereas the one with a lower Ni charge-state and more NiSe 2 phase boosts hydrogen evolution reaction (HER). Density functional theory calculations reveal that the interfacial electrons transfer from Ni 3 Se 4 to NiSe 2 , which improves conductivity and optimizes adsorption/desorption energies. NiSe 2 /Ni 3 Se 4 /NF-4 containing more NiSe 2 phase displays the best HER activity while NiSe 2 /Ni 3 Se 4 /NF-1 containing more Ni 3 Se 4 phase shows the best HER activity. The electrolyzer, employing NiSe 2 /Ni 3 Se 4 /NF-4 and NiSe 2 /Ni 3 Se 4 /NF-1 as the cathode and anode, respectively, performs the full potential and demonstrates a low voltage of 1.56 V achieving 10 mA cm −2 with good durability.
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Materials Today Chemistry
·
2021
·
IF 8.301
X. Xia,J. Shi,Q. Deng,N. Xu,F. Huang,X. Xiang
Mesoporous organosilica as drug delivery carriers capable of achieving improved cargo release, enhanced biodegradation, and direct imaging with prolonged circulation time and tracking cargo distribution is highly in demand for biomedical applications. Herein, we report a ditelluride-bridged mesoporous organosilica nanoparticle (DTeMSN)/polyethylene glycol-curcumin (PEG-CCM) nanocomposite through coassembly with oxidative/redox and self-fluorescent response. Tellurium is introduced into the silica framework for the first time as a drug delivery vehicle. In this case, the DTeMSNs as an inner core enable disassembly under oxidative and redox conditions via the cleavage of ditelluride bond, facilitating the drug release of doxorubicin (DOX) in a matrix degradation controlled manner. Through the systematical comparison of diselenide-bridged MSNs and DTeMSNs, DTeMSNs exhibit remarkable advantages in loading capacity, drug release, and degradation behavior, thereby significantly affecting the cytotoxicity and antitumor efficacy. The self-fluorescent response of PEG-CCM shell coated on the surface of DTeMSNs can real-timely track the cellular uptake, DOX release, and biodistribution owing to the intrinsic and stable fluorescence of CCM. Moreover, PEG-CCM could prolong circulation time, provide preferable drug accumulation in tumors, and increase antitumor efficacy of DOX-loaded DTeMSNs. Our findings are likely to enrich the family of organosilica that served as fluorescence-guided drug delivery carriers.
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CHEMOSPHERE
·
2021
·
IF 7.086
Liangmei Rao,Xinyu Lu,Lulu Xu,Yifu Zhu,Ting Xue,Yu Ge,Zhongshu Duan,Xuemin Duan,Yangping Wen,Jingkun Xu
It is an urgent need to exploit a potentially green, cost efficient and eco-friendly strategy for the utilization of waste kudzu vine. We developed a one-step green preparation of kudzu vine biochar (BC) decorated graphene-like molybdenum selenide (MoSe 2 ) with the oxidase-like activity as intelligent nanozyme sensing platform for voltametric detection of hesperetin (HP) in orange peel using the in-situ hydrothermal synthesis method. The structure and properties of MoSe 2 -BC was characterized, and found that BC significantly improved electrochemical cycle stability, electronic conductivity, electrochemical active area, and electrocatalytic activity of MoSe 2 . The oxidase-like activity of MoSe 2 -BC was confirmed by the oxidization of the colorless substrate 3,3′,5,5′-tetramethylbenzidine (TMB) to form blue products and the change of absorbance intensity of UV–vis absorption spectra . The MoSe 2 -BC exhibited excellent electrochemical sensing performance for the detection of HP in wide linear ranges from 10 nM to 9.5 μM with a low limit of detection of 2 nM using differential pulse voltammetric method. An emerging machine learning technique is used to realize the intelligent sensing of HP, and the performance evaluation of regression analysis was selected to evaluate this technique. This work will provide a guidance for the preparation and application of biochar decorated graphene-like nanomaterials with the oxidase-like activity and the development of intelligent nanozyme sensing platform.
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MATERIALS CHEMISTRY AND PHYSICS
·
2021
·
IF 4.094
Yinggang Liu,Shuai Liu,Hanxiao Li,Lijun Yu,Lan Sun,Jiale Xue,Ruojun Xu,Guoxiang Chen
Transition metal dichalcogenides (TMDCs) are considered as the potential electrocatalysts for hydrogen evolution reaction (HER) owing to the two-dimensional (2D) geometry and tunable band gap. However, both the inefficient electron transferring and high Gibbs free energies for hydrogen adsorption (ΔG H *) in MoSe 2 limit its further improvement in catalytic performance. Herein, the few-layered 1T@2H–MoSe 2 composite nanosheets are synthesized by one-pot hydrothermal reaction . It is found that the morphology and composites of nanosheets could be influenced by hydrothermal reaction parameters. As compared to pure 2H–MoSe 2 , 1T@2H–MoSe 2 electrode exhibits remarkable activity for HER with a low overpotential (118 mV), small Tafel slope (65.8 mV·dec −1 ) as well as large electrochemical active area (C dl = 37.5 mF cm −2 ) in acid electrolytes. Density functional theory (DFT) calculations demonstrate that ΔG H * of 1T@2H–MoSe 2 (0.232 eV) is much lower than these of pure 1T-MoSe 2 and 2H–MoSe 2 . It could be ascribed to both the optimized charge transfer and increased density of active sites in 1T@2H–MoSe 2 nanosheets.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
·
IF 5.316
Yi Wang,Xinyan Xiao,Mingli Lu,Yu Xiao
The transition-metal dichalcogenides (TMDs) is a promising photocatalyst for degrading contaminant, while limited active sites and poor carrier mobility are the primary challenges for improving photocatalytic degrading efficiencies in both bare TMDs and TMDs-based photocatalysts. A rGO-MoSe 2 composite with 3D network hierarchical structure was fabricated by the GO-assisted solvothermal method. And then rGO-MoSe 2 /g-C 3 N 4 3D/2D hierarchical structures were constructed by combining rGO-MoSe 2 with g-C 3 N 4 nanosheets . The optimal rGO-MoSe 2 /g-C 3 N 4 composite exhibited the highest photocatalytic degrading rate of 97.4% towards RhB under simulated solar light, and its pseudo-first-order apparent rate constant ( k ) was 0.0715 min −1 , being 5.9 and 12.5-folds higher than that of MoSe 2 /g-C 3 N 4 (0.0121 min −1 ) and bare g-C 3 N 4 (0.00573 min −1 ), respectively. The 3D/2D hierarchical structure endow rGO-MoSe 2 /g-C 3 N 4 composite with the improved light-harvesting and abundant active sites, supported by the DRS and BET analyses. And rGO nanosheets could act as efficient transfer and separation channels for electron-hole pairs between MoSe 2 and g-C 3 N 4 , confirmed through the photocurrent response and EIS tests. According to the results of DRS spectra and Mott-Schottky plots, the spatial behavior of photo-induced carriers at interface of rGO-MoSe 2 /g-C 3 N 4 would comply to a Z-scheme transfer pathway under the synergy effects of the internal electric field and band bending.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Xue Zhang,Chuanjun Xi,Yuanhang Yue,Puhui Deng,Linping Zhang,Yu Hou
Seeking an efficient and non-precious co-catalyst for g-C 3 N 4 (CN) remains a great demanding to achieve high photocatalytic hydrogen generation performance. Herein, a composite photocatalyst with high efficiency was prepared by modifying CN with coral-like NiSe 2 . The optimal hydrogen evolution rate of 643.16 μmol g −1 h −1 is from NiSe 2 /CN-5 under visible light. Superior light absorption and interfacial charge transfer properties including suppressed photogenerated carrier recombination and efficient separation of photogenerated electron-hole pairs have been observed, which account for the enhanced photocatalytic performance of CN.
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Foods
·
2021
·Vol. 10
·期 11
·2810
·
IF 4.35
Xinpeng Yan,Zhong Zhang,Runguang Zhang,Tian Yang,Guoying Hao,Li Yuan,Xingbin Yang
Given the imperative of monitoring organophosphorus pesticides (OPs) residues in the ecosystem, here a novel, facile and sensitive fluorescence sensor is presented for the rapid detection of dimethoate. In this work, surface molecularly imprinted polymer (SMIP) and microfluidic technology had been introduced to enhance the selectivity and portability of the described methodology. Oil-soluble CdSe quantum dots (QDs) synthesized in a green way were used as fluorescent material for the selective detection of dimethoate on the basis of static quenching and photoinduced electron transfer mechanism. Among many kinds of paper materials, glass fiber paper was used as the novel substrate of paper chip due to low pristine fluorescence and better performance when combining CdSe QDs. In the process of molecular imprinting, the interaction between several functional monomers and dimethoate molecule was investigated and simulated theoretically by software to improve the selectivity of the sensor. Consequently, the fabricated novel detection platform could effectively respond to dimethoate in 10 min with the concentration range of 0.45–80 μmol/L and detection limit of 0.13 μmol/L. The recovery in the spiked experiment soybean sample was in an acceptable range (97.6–104.1%) and the accuracy was verified by gas chromatography-mass spectrometry, which signified the feasibility and potential in food sampling.Keywords:oil-soluble CdSe QDs;dimethoate;microfluidic paper chip;fluorescence sensor
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Weiji Dai,Yin'an Zhu,Yike Ye,Ye Pan,Tao Lu,Saifang Huang
Surface reconstruction of non-oxide oxygen evolution reaction (OER) electrocatalysts has been intensively studied to improve their catalytic performances. However, further modification of the reconstructed active surfaces for better catalytic performances has not been reported. In this work, NiSe nanorods are prepared on nickel foam (NiSe@NF) as the pre-catalyst for electrochemical OER. It is revealed that non-stoichiometric NiO nanosheets with abundant Ni vacancies (Ni x O) are formed on the surfaces of NiSe nanorods (Ni x O/NiSe@NF) via in-situ electrochemical oxidation. Furthermore, the OER performances are obviously improved after heteroatom Fe is incorporated electrochemically into Ni x O nanosheets ((FeNi)O/NiSe@NF). For OER to have a current density of 20 mA cm −2 in 1 M KOH solution, the as-prepared (FeNi)O/NiSe@NF electrode only needs an overpotential of 268 mV. Density functional theory (DFT) calculations reveal that the formation of Ni vacancy can increase the free energy of *OH. More importantly, the incorporation of heteroatom Fe into Ni vacancy can significantly decrease the free energy of *O, which enables Fe-NiO to have the lowest theoretical overpotential for OER in this work. The present work provides a facile and universal strategy to modify the reconstructed active oxides’ surfaces for higher electrocatalytic performances.
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ADVANCED MATERIALS
·
2021
·Vol. 34
·期 3
·2106502
·
IF 30.849
Jia-Xin Yu,Shuai Xing,Guang-Yu Dai,Shuang-Yi Ling-Hu,Fu-Xing Gu
Monolayer transition metal dichalcogenides (TMDs) have emerged as widely accepted 2D gain materials in the field of light sources owing to their direct bandgap and high photoluminescence quantum yield. However, the monolayer medium suffers from weak emission because only a single layer of molecules can absorb the pump energy. Moreover, the material degradation when transferring these fragile materials hinders their cooperation with the optical cavity further. In this study, for the first time, a high-quality monolithic structure is developed by directly growing single-domain tungsten diselenide (WSe 2 ) bilayers on single silica microsphere (MS) cavities. Such a completely wrapped structure guides the indirect-to-direct bandgap transition of WSe 2 bilayers, leading to a significantly improved photoluminescence intensity by about 60-fold. Moreover, the high-quality monolithic structure enhances the confinement factor of the cavity by more than 20-fold. Based on the above advantages, a bilayer WSe 2 /MS microlaser is realized with an ultralow threshold of 0.72 W cm −2 , nearly an order of magnitude lower than the existing records. The results demonstrate the possibility of using multilayer TMD materials as 2D gain media and provide insights into a new ultracompact monolithic platform of TMD material/cavity for lasing devices.
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