INORGANIC CHEMISTRY
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2022
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IF 5.436
Mianmian Wu,Nan Li,Shixiang Zuo,Wenjing Shen,Guifang Sun,Qingfei Li,Minghao Shi,Jiangquan Ma
Piezocatalysis is a promising technology to address environmental pollution by converting mechanical energy into chemical energy. Herein, MoSe2 nanosheets with different 1T phase percentages (ranging from 30 to 80%) were constructed by adjusting hydrothermal temperature. Moreover, the roles of phase engineering in the piezocatalysis were thoroughly investigated by degrading rhodamine B and reducing Cr(VI) in ultrasonic vibration conditions. In particular, MoSe2 prepared at 220 °C (MoSe2-220) exhibits ultrahigh observed constant kobs and degradation rate k, which is superior to most reported catalysts to date. The experimental results indicate that the introduction of the 1T phase increases the active sites of the material, improves the conductivity, and inhibits the recombination of electrons and holes. Moreover, an internal electric field in the 2H phase induced by piezoelectric polarization is facilitated to separate electron–hole pairs, enabling the degradation and reduction to proceed. The capture experiments and EPR tests further confirm that •O2– and •OH are main reactive species, and a rational mechanism is finally put forward. This study offers a clear understanding of phase engineering in piezocatalysis and provides an efficiency strategy to construct highly efficient piezocatalysts.
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高影响因子
TALANTA
·
2022
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IF 6.556
Shan He,Wen-Le Fang,Xiao-Feng Guo,Hong Wang
Redox homeostasis is the guarantee for the normal operation of living organisms. Given its importance, monitoring dynamic changes of redox state will facilitate the study of relevant physiological and pathological processes. Herein, a two-photon fluorescent probe NA-Se with selenomorpholine as the response site has been developed for reversible detection of redox state. NA-Se exhibits outstanding analytical performance, including a rapid response to ClO − within 8 s, a detection limit as low as 13.3 nM, and at least 10 redox reversible cycles. Furthermore, NA-Se has improved water solubility and extremely low cytotoxicity, making it ideal for bioimaging. Finally, NA-Se has been successfully applied to monitor the ClO − /GSH redox cycle in living cells and zebrafish. This work may provide an effective tool for studying redox state and related diseases in vivo.
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IONICS
·
2022
·Vol. 29
·期 1
·313-322
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IF 2.961
Xu Xiaoxuan,Li Chen,Li Na,Zhong Jiajin,Wang Xing,Fang Zheng,Bao Haifeng
Nickel-based selenides have attracted widespread attention as promising electrocatalysts for water splitting. This work proposes a novel and facile method to fabricate an efficient electrocatalyst based on morphological controlled nickel diselenide nanoparticles using L-cysteine (NiSe 2 -L) via atmospheric pressure hydrothermal. The NiSe 2 -L was prepared inside a round-bottom flask under stirring conditions in an oil bath at 100 ℃ for 4 h. This method no longer required posttreatment, just used L-cysteine for morphological control, and the reaction time was shortened to only 4 h. As expected, the NiSe 2 -L electrode exhibited good catalytic performance towards oxygen evolution reaction (OER) with an overpotential of 398 mV at the current density of 100 mA cm −2 and maintained a Faraday efficiency of up to 99% in 1 M KOH. Moreover, this electrode showed long-term stability with small overpotential increases (~ 16 mV) at 100 mA cm −2 after 5000 cycles of CV scans. Therefore, this work provided a facile synthesis method of nickel-based selenides with potential use value for OER in alkaline solutions.
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Nature Photonics
·
2023
·Vol. 17
·期 4
·346-353
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IF 35
Liang Wenfei,Nie Chengming,Du Jun,Han Yaoyao,Zhao Guohui,Yang Fan,Liang Guijie,Wu Kaifeng
Near-infrared-to-visible photon upconversion holds great promise for a diverse range of applications. Current photosensitizers for triplet-fusion upconversion across this spectral window often contain either precious or toxic elements and have relatively low efficiencies. Although colloidal nanocrystals have emerged as versatile photosensitizers, the only family of nanocrystals discovered for near-infrared upconversion is the highly toxic lead chalcogenides. Here we report zinc-doped CuInSe 2 nanocrystals as a low-cost and lead-free alternate, enabling near-infrared-to-yellow upconversion with an external quantum efficiency reaching 16.7%. When directly merged with photoredox catalysis, this system enables efficient near-infrared-driven organic synthesis and polymerization, which in turn solves the issue of reabsorption loss for nanocrystal-sensitized upconversion. Moreover, the broadband light capture of these nanocrystals enables very rapid reactions under indoor sunlight. Extending the reach of ‘solar synthesis’ into the near-infrared may realize the century-long dream of conducting high-added-value chemical transformations using sunlight.
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Journal of Energy Storage
·
2022
·
IF 8.907
Tao Cui,Shang Wu,Sheng Zhou,Qiaoliang Feng,Xin Xu,Huanlei Zhao,Qiong Su,Yanbin Wang,Xiangfei Zhao,Quanlu Yang
The core-shell structure is always a greatly effective structure in asymmetric hybrid supercapacitor , duo to a high specific surface area and porosity that can accommodate partial expansion during the redox reaction. Herein, a cobalt-glycerolate@nickel hydroxidenitrate microsphere (CoG@Ni 3 (NO 3 ) 2 ·(OH) 4 ) with core-shell structure is prepared by a simple two-step hydrothermal method . The as-produced CoG@Ni 3 (NO 3 ) 2 ·(OH) 4 possesses extremely high specific capacity (265.9 mA h g −1 at 1 A g −1 ) and an excellent rate capability (with 75.5% of initial capacity at 10 A g −1 ). In addition, as an cathode material, flower-sphere-like Bi-Bi 2 Se 3 materials is selected to match a new CoG@Ni 3 (NO 3 ) 2 ·(OH) 4 //Bi-Bi 2 Se 3 asymmetric supercapacitor. It exhibits a specific capacity (125.1 mA h g −1 at 1 A g −1 ) and an impressive rate property (with 77.6% of initial capacity at 10 A g −1 ). Satisfactorily, the asymmetric supercapacitor device, which cleverly assembles by the above two electrode materials, achieves impressive specific energy of 54 Wh kg −1 at 760 W kg −1 , and a capacitance retention rate of 80% after 4000 cycles. The excellent performance of the asymmetric supercapacitor proves that the materials possess great potential in the energy storage field.
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SENSORS AND ACTUATORS B-CHEMICAL
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2022
·
IF 9.221
Yihan Wang,Jinfeng Quan,Jialei Zhang,Kejing Huang,Xuemei Wang,Hui Jiang
The fragments of molecular motors can be transported and operated autonomously along a track. Most molecular walker systems are assembled from DNA building modules, exhibiting great potential applications in biocomputing, drug transport, sensing, etc. Hereby, we report a DNA walker driven by endonuclease Nt.BbvC I that can autonomously induce “signal off” sensing platform for highly sensitive detection of tumor cells. DNA density and trajectory conformation can affect DNA walker properties. Molybdenum selenide@gold nanoparticles (MoSe 2 @AuNPs) are modified on the electrode surface as a scaffold to accommodate more hairpin probe (H1) and provide a good interface for DNA walking. Magnetic beads are used to enrich target tumor cells, release single-stranded DNA (S1) and trigger DNA walker-based amplification strategy. Upon addition of tumor cells, more DNA-methylene blue (DNA-MB) is cracked from the electrode surface. Benefiting from efficient electrode modification, magnetic enrichment, DNA walker and enzyme-assisted amplification, an ultra-high sensitivity electrochemical cell analysis is realized, with a detection limit of 2 cells mL −1 . More importantly, this DNA walker strategy is available for tumor cell analysis in clinical samples, suggesting the potential diagnostic applications.
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MATERIALS & DESIGN
·
2022
·
IF 9.417
Yanbin Zhang,Lu-Lu Qiao,Zhi-Qiang Zhang,Yong-Fang Liu,Lin-Song Li,Huaibin Shen,Mei-Xia Zhao
Numerous cellular functions are closely reliant on mitochondria and so the capability to conduct long-term stable studies of their activity is of great importance. However, current commercial mitochondrial probes are severely limited in their ability to trace mitochondria due to their inherently poor stability. Here, for the first time, we designed a novel mitochondrial fluorescent probe using InP quantum dots (QDs) as a fluorescent master and skillfully combined with (3-carboxypropyl)triphenylphosphine (TPP) for specific recognition. The bespoke InP QDs probes described here exhibited clear advantages, including simple and low-cost synthesis, high quantum yields, extremely low toxicity, good biocompatibility, and excellent photochemical stability, thus representing a versatile, novel mitochondrial fluorescent probe, particularly suitable in applications traditionally undertaken by Cd-based QDs in biological fields.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2022
·
IF 5.876
Zhiqiang Zhou,Yuanping Liao,Huiyan Wu,Qi Xiao,Yi Liu,Liyun Yang
Herein, zeolitic imidazolate framework-8 capped gold nanoclusters (AuNCs@ZIF-8) was fabricated and developed as an “on-off-on” fluorescent nanoprobe for selectively and sensitively detecting KMnO 4 and ascorbic acid (AA). The prepared AuNCs@ZIF-8 initially exhibited strong fluorescence at 595 nm KMnO 4 could quench the fluorescence of AuNCs@ZIF-8, rendering the fluorescence signal of AuNCs@ZIF-8 in the “off” state. The probe allows KMnO 4 to be detected with a 10 nM detection limit and the linear analytical range was 0.05–2 μM. When AA was added into the AuNCs@ZIF-8/KMnO 4 system, the fluorescence of the AuNCs@ZIF-8 recovered due to the redox reaction between KMnO 4 and AA, and the fluorescence signal of the system turned “on”. The detection limit of AA was 37 nM in a good linear concentration range of 0.05–5 μM. Furthermore, this AuNCs@ZIF-8 nanoprobe was successfully used for AA detecting in fresh orange juices with the recoveries ranged from 96.6% to 108.2%, which validates the potential applicability of this strategy.
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COLLOIDS AND SURFACES B-BIOINTERFACES
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2022
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IF 5.999
Liangjie Shi,Yong Jin,Shuangquan Lai,Long Bai,Rong Zhou,Yutang Zhou,Xiang Shang
Polymeric micelle has emerged as an efficient implement to overcome the shortcomings of conventional cancer chemotherapy due to its superior solubility of hydrophobic drugs and less side effects of drugs. However, insufficient dilution resistance and ordinary therapeutic effect severely restrict the further translation of current drug-loaded polymeric micelles. Here, we showed that well-defined G-Fn (n = 5, 9, 13) polymeric micelles possessed excellent capabilities as a drug carrier in light of high drug loading content, high stability and precise drug release combined with wonderful endocytosis efficiency to tumors. The representative G-F13 exhibited an excellent dilution resistance, outstanding high drug loading content (22 wt%) and drug loading efficiency (82%), which might be attributed to the extremely low critical micelle concentration conferred by its special Gemini structure and the superhydrophobicity of the fluorocarbon chain. Furthermore, the “cross-linked” internal fluoride membrane consisted of the two chains of the Gemini structure made G-F13 stable even after 24 h of incubation in 10% fetal bovine serum (FBS). The camptothecin (CPT) release was selectively triggered by glutathione (GSH) and H 2 O 2 , reaching 75% and 85% after 24 h respectively, in which only 15% of drugs leak under physiological conditions. The CCK-8 assays of Hela cells showed that CPT-loaded G-F13 micelles had high cell compatibility (200 μg/mL, 93% cell viability , 48 h) and high cancer cytotoxicity (IC50 0.1 μg/mL). Notably, a tenfold lower dosage of loaded CPT had an higher tumor growth inhibition than the free CPT. This result was attributed to the combined treatment of fluorinated drug carriers were more likely to penetrate the cell membrane to enter tumor cells, the cytotoxicity of selenic acid generated after the oxidation of G-F13 and the large amounts of CPT after redox release. Excellent physical and chemical properties as well as good therapeutic effects reveal that G-F13 can act as a promising drug carrier to widely use in cancer chemotherapy.
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JOURNAL OF PHYSICS AND CHEMISTRY OF SOLIDS
·
2022
·
IF 4.383
Mehboob Hassan,Mirza Mahmood Baig,Khalid Hussain Shah,Aftab Hussain,Syeda Aqsa Hassan,Arshad Ali
The synthesis of an economical and efficient bifunctional electrocatalyst for general water splitting is necessary for the fabrication of eco-friendly H 2 energy. Herein, state-of-the-art ZIF-67-based CoSe/MoSe 2 hybrid nanospheres were synthesized and examined as a bifunctional electrocatalyst for Hydrogen evolution reaction (HER) and Oxygen evolution (OER) in basic media. For the first time, a hierarchical well-designed CoSe/MoSe 2 hybrid nanospheres designed with the uniform distribution layered of 2D-MoSe 2 and conductive CoSe nanoparticles are acquired from CoMoO 4 via selenization. Due to its large surface area and extraordinary morphology, it exhibited significant catalytic activity, which leads to a small overpotential of 110 mV for HER and for 240 mV OER along with low Tafel values of 54.24 and 51.98 mV dec −1 , respectively. Surprisingly, the stability is marvelous and also comparable to the standard of HER and OER. The enhancement is endorsed by the increase in conductivity evolved from the porous nanospheres and the collaborative effect of Co/Mo. To deliver a current density of 10 mA per cm 2 for full water splitting 1.56 V is required, which is one of the least reported voltages. Therefore, this work leads to a new class of catalysts for the fabrication of an efficient water electrolyzer.
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ACS Applied Energy Materials
·
2022
·
IF 6.959
Yuping Che,Bingxin Lu,Huaxiang Chen,Jin Zhai,Kefeng Wang,Huaiqiu Chang,Zhaoyue Liu
Adding a cocatalyst to a semiconductor catalyst is often considered an effective measure to increase the efficiency of the photocatalytic hydrogen evolution reaction. Nowadays, noble metals are the state-of-the-art cocatalysts for the hydrogen evolution reaction. Due to their high cost and scarcity, it is imperative to develop cocatalysts prepared from cheap and abundant elements. Here, RuSe2 was used as an effective substitute for precious metal promoters such as Pt to enhance the efficiency of g-C3N4 for the hydrogen evolution reaction. A high efficiency of 13417.3 μmol·g–1·h–1 was obtained. It was 214 times higher than that of g-C3N4 and 2.8 times higher than that of 3%Pt/g-C3N4. Density functional theory calculations were performed. The (210) and (200) crystal faces of RuSe2 showed lower ΔGH* than Pt(111), indicating higher hydrogen evolution efficiency. Compared with the Pt cocatalyst, metallic RuSe2 cocatalysts exhibited superior performance. Meanwhile, the electrocatalytic activity was also investigated in an alkaline medium. It showed a decent electrocatalytic activity and high stability. These findings might provide a prototype to develop cheap and efficient cocatalysts for large-scale water splitting.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Jean Pierre Mwizerwa,Changyong Liu,Kun Xu,Ning Zhao,Zhangwei Chen,Jun Shen
Surface engineering of transition metal oxide cathode materials for Li-ion batteries is highly important to achieve high-capacity retention, high-rate capability, and long-life term. In this study, VSe 2 nanosheets are prepared and used as a surface sensitizer to enhance the electrochemical properties of LiFePO 4 (LFP) cathode material. The LiFePO 4 @VSe 2 (LFP@VSe 2 ) composite is formed by anchoring 1D-LFP particles with the as-prepared 2D-VSe 2 nanosheets by using an in-situ solution phase technique. When the LFP@VSe 2 composites are used as cathode materials for Li-ion batteries, the Li surface-controlled storage behavior of the batteries is reasonably enhanced. The performance is attributed to the improvement in the inherent Li-ion conductivity of LFP particles, thereby inhibiting surface diffusion drawbacks and decreasing charge transfer resistance. The exterior VSe 2 attached to the LFP serves as a second electrically conducting layer to increase conductivity into the entire electrode. Thus, these conditions enhance the electron transfer kinetics and surface stability of the LFP cathode. LFP@VSe 2 composite cathode exhibits an ultrastable specific capacity of 166.5 mAh g −1 after 100 cycles @ 0.1 C and can retain a specific capacity of 146.7 and 46.5 mAh g −1 after 700 and 2000 cycles respectively at a current rate of 0.3 C and 10 C.
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