APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Yingtong Zou,Yezi Hu,Andrej Uhrich,Zewen Shen,Baoxiang Peng,Zhuoyu Ji,Martin Muhler,Guixia Zhao,Xiangke Wang,Xiaoxiang Xu
We provide a distinct understanding on the role of oxygen vacancies (OVs) for visible light-triggered aerobic oxidation of alcohols via comparative studies on three kinds of Nb 2 O 5 , i.e., undoped, Ti-doped and Ce-doped Nb 2 O 5 . With benzyl alcohol and 5-hydroxymethylfurfural as representative alcohol substrates, we show that fast alcohol oxidation with high selectivity can be achieved on these doped Nb 2 O 5 containing abundant OVs. However, the functionality of OVs is dependent on the properties of dopants as Ce-doped Nb 2 O 5 exhibits a better performance than Ti-doped one. Investigations indicate that the Ce dopants incur little distortion to the structure of Nb 2 O 5 and induce more accessible OVs than Ti dopants for the dissociative chemisorption of alcohol molecules which supports favorable interfacial electron migration process. The present work not only reveals the difference of oxygen vacancies caused by varied metal doping but provides a unique insight in the relation between OVs structure and photocatalytic alcohol oxidation.
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MACROMOLECULAR MATERIALS AND ENGINEERING
·
2021
·Vol. 306
·期 9
·2100106
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IF 4.367
Yue Ma,Yuman Yang,Daruo Cao,Jun Fang,Cheng Zhu,Meng Yang,Liang Fang,Chunhua Lu,Zhongzi Xu
Photothermally induced self-healing coatings are widely reported, while their application scenarios are rarely taken with concern. In addition, there is a need to achieve the balance between good properties and self-healing behaviors for closing the gap between academic research and engineering applications. Here, self-healing composite coatings are designed based on silane-modified epoxy chains with reversible crosslinking points and multifunctional fillers of cerium oxide nanoparticles grown on graphene nanosheets, and their applications are demonstrated for restricted regions. Diglycidyl ether-terminated poly(dimethylsiloxane) is co-polymerized with diglycidylether of bisphenol A with the weight ratio of 1/99–10/90 to achieve surface-tension driven crack closure, while dangling furan groups contribute to reversible crosslinking points via Diels–Alder reaction. Cerium oxide nanoparticles and graphene nanosheets enhance anti-corrosion properties, and graphene nanosheets also act as photothermal fillers. The results show that pencil hardness, polarized resistance, and coating resistance are highly improved via the introduction of multifunctional fillers at 1 and 2 phr. Good thermally and photothermally induced self-healing is demonstrated. This work provides a new application thought for light triggered self-healing coatings that can be used for restricted regions including inner walls of pipelines and reactors.
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ACS Catalysis
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2021
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IF 13.084
Yong Xu,Xuchun Wang,Di Yang,Zeyuan Tang,Muhan Cao,Huicheng Hu,Linzhong Wu,Lijia Liu,John McLeod,Haiping Lin,Youyong Li,Yeshayahu Lifshitz,Tsun-Kong Sham,Qiao Zhang
The conversion of light alkanes to olefins (e.g., ethylene, propylene, or butylene) is crucial to the chemical industry. ZrO2 with oxygen vacancies has recently been regarded as a promising catalyst for the direct dehydrogenation of light alkanes. However, the intrinsic mechanism of the effect of oxygen vacancies on catalytic performance has not been completely understood yet, and ZrO2 without promoters generally displays poor activity toward the direct dehydrogenation of light alkanes. In this work, we demonstrate that the oxygen vacancies in ZrO2 can be poisoned by H atoms during the dehydrogenation of light alkanes, and we report a strategy for stabilizing the oxygen vacancies in ZrO2 by Ga2O3. Experimental results and theoretical calculations indicate that ZrO2 with oxygen vacancies is responsible for dehydrogenation, while Ga2O3 prevents the poisoning of oxygen vacancies by dissociated hydrogen atoms which, in the absence of the Ga2O3 component, blocks further dehydrogenation. Consequently, the optimal Zr0.26Ga1 catalyst exhibits superior propane dehydrogenation performance to the industrial Pt–Sn catalyst, the state-of-the-art catalyst for the direct dehydrogenation of light alkanes. We anticipate this work may shed light on both the fundamental research of catalysis and the chemical industry.
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Materials Horizons
·
2021
·Vol. 8
·期 11
·3063-3071
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IF 13.266
Hongtai Ren,Hu Jin,Jian Shu,Jie Xie,Erlong Wang,Du-An Ge,Shi-Yang Tang,Xiangpeng Li,Weihua Li,Shiwu Zhang
The controlled actuation of liquid metal (LM) droplets has recently shown great potential in developing smart actuating systems for applications in robotics. However, there is a lack of a simple approach for the precise manipulation of multiple LM droplets in a 2D plane, which hinders the development of complex control over droplets for realizing useful robotic applications. To overcome this challenge, here, a versatile and powerful light-induced manipulation of LM droplets is presented. The key principle is to selectively activate phototransistors in an electrolyte using infrared laser beams to electrically control LM droplets via Marangoni forces. This approach shows the ability of inducing concurrent motion, splitting, and merging of multiple LM droplets simply using light without complex and bulky systems. Parameters affecting the manipulation of LM droplets are thoroughly investigated. Moreover, a vehicle carrier driven by wheels composed of multiple LM droplets for making a light-controlled relay is demonstrated. We believe such a light-induced control method for manipulating LM droplets has the potential for advancing the development of future field-programmable robotics and droplet-based soft collaborative robots.
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Frontiers in Chemistry
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2021
·
IF 5.221
Wu Mingzhou,He Shuqing,Hu Xin,Chen Jingqin,Ha Enna,Ai Fujin,Ji Tao,Hu Junqing,Ruan Shuangchen
Transition-metal chalcogenide compounds with facile preparation and multifunctional elements act as ideal photothermal agents for cancer theranostics. This work synthesizes Cu7.2S4/5MoS2 composite nanoflowers and investigates the crystal growth mechanism to optimize the synthesis strategy and obtain excellent photothermal therapy agents. Cu7.2S4/5MoS2 exhibits a high photothermal conversion efficiency of 58.7% and acts as a theranostic nanoplatform and demonstrated an effective photothermal–chemodynamic–photodynamic synergetic therapeutic effect in both in vitro and in vivo tests. Moreover, Cu7.2S4/5MoS2 shows strong photoacoustic signal amplitudes and computed tomographic contrast enhancement in vivo. These results suggest a potential application of Cu7.2S4/5MoS2 composite nanoflowers as photo/H2O2-responsive therapeutic agents against tumors.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Yawei Jiang,Yan Mi,Chufan Li,Wenjian Fang,Xiaochuan Li,Xianghua Zeng,Yongsheng Liu,Wenfeng Shangguan
The solid solution constructed by two or more semiconductors with different bandgaps can effectively modulate the energy band, satisfying the redox potential for both H + /H 2 and O 2 /H 2 O. In this paper, Sillen-Aurivillius compounds with layered structure Bi 3 O 4 Cl and Y 3 O 4 Cl solid solution (Bi 3−x Y x O 4 Cl) were successfully synthesized by the solid-phase method. The absorption edge of Bi 3−x Y x O 4 Cl could be dramatically changed from about 500–740 nm with the increase of Bi elements, which accounted for the entire UV-Vis region of the solar spectrum. Furthermore, the bandgaps for Bi 3−x Y x O 4 Cl could be adjusted from about 2.6–2.0 eV with the decreased Y/Bi ratio from 2 to 0.2. Significantly, the conduction band minimum energy (CBM) of Bi 3−x Y x O 4 Cl all satisfied the redox potential for H + /H 2 , which showed excellent visible-light photocatalytic water splitting.
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JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2021
·
IF 8.067
Bing Leng,Xinglai Zhang,Shanshan Chen,Jing Li,Ziqing Sun,Zongyi Ma,Wenjin Yang,Bingchun Zhang,Ke Yang,Shu Guo
The development of high-efficiency photocatalysts is the primary goal in the field of photocatalytic antibacterial research. In this work, the GaN:ZnO solid solution nanoparticles (NPs) photocatalyst with strong visible absorption and large specific surface area was synthesized via the sol-gel and nitridation reaction process. Also, we systematically investigated the removal efficiency of the organic pollutant and antibacterial activity on E. coli and S. aureus . Notably, methylene blue solution could be completely degraded after 100 min of visible light illumination using 2 mg/mL GaN:ZnO catalyst. Moreover, ~94% of the E. coli were inactivated within 120 min, whereas 100% antibacterial activity against S. aureus was achieved after 90 min of visible light illumination mediated by GaN:ZnO NPs. We further explore the potential mechanism of visible light photocatalytic antibacterial activity enhanced by GaN:ZnO NPs photocatalyst. The current work not only provides a new and efficient photocatalytic antibacterial nanomaterial but also demonstrates its promising applications in environmental and biological fields.
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ACS Nano
·
2021
·
IF 15.881
Xueting Zhai,Renxiang Zhang,Huixiang Sheng,Jin Wang,Yameng Zhu,Zichen Lu,Zhuoyao Li,Xiao Huang,Hai Li,Gang Lu
Single and a few atomic-layer molybdenum disulfide (MoS2) is a promising material in the fields of hydrogen generation, battery, supercapacitor, and environmental protection, owing to the outstanding electronic, optical, and catalytic properties. Although many approaches have been developed for exfoliation of MoS2 sheets, it is still essential to develop simple, convenient, and environmental friendly exfoliation methods. More importantly, the microscopic exfoliation process and the mechanism are still not clear, limiting a deeper understanding of the exfoliation. Herein, we develop a convenient and clean method for exfoliation of the 2H phase MoS2 (2H-MoS2) deposited on an indium tin oxide (ITO) surface. Importantly, the exfoliation process is observed directly and continuously under an optical microscope to reveal the detailed exfoliation process and mechanism. As illustrated, the light illumination triggers the exfoliation of the 2H-MoS2 sheets, and the presence of water is essential in this exfoliation process. The light intensity and wavelength, humidity, and bias all affect the exfoliation process obviously. The exfoliation is caused by the vaporization of the water molecules intercalated in 2H-MoS2 interlayers. By using this method, 2H-MoS2 nanosheets with different thicknesses are prepared on the ITO substrate, and microscopic catalysis mapping of the exfoliated sheets is demonstrated with single-molecule fluorescence microscopy, revealing that the prepared thin-layer 2H-MoS2 nanosheets show improved electrocatalysis activity (roughly 20 times). Our work will not only help deepen the understanding of exfoliation process of two-dimensional nanosheets but also provide an effective tool for the in situ study of various properties of the exfoliated sheets.
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ADVANCED MATERIALS
·
2021
·Vol. 33
·期 18
·2007169
·
IF 30.849
Zema Chu,Qiufeng Ye,Yang Zhao,Fei Ma,Zhigang Yin,Xingwang Zhang,Jingbi You
Perovskite light-emitting diodes (PeLEDs) are considered as particularly attractive candidates for high-quality lighting and displays, due to possessing the features of wide gamut and real color expression. However, most PeLEDs are made from polycrystalline perovskite films that contain a high concentration of defects, including point and extended imperfections. Reducing and mitigating non-radiative recombination defects in perovskite materials are still crucial prerequisites for achieving high performance in light-emitting applications. Here, ethoxylated trimethylolpropane triacrylate (ETPTA) is introduced as a functional additive dissolved in antisolvent to passivate surface and bulk defects during the spinning process. The ETPTA can effectively decrease the charge trapping states by passivation and/or suppression of defects. Eventually, the perovskite films that are sufficiently passivated by ETPTA make the devices achieve a maximum external quantum efficiency (EQE) of 22.49%. To our knowledge, these are the most efficient green PeLEDs up to now. In addition, a threefold increase in the T 50 operational time of the devices was observed, compared to control samples. These findings provide a simple and effective strategy to make highly efficient perovskite polycrystalline films and their optoelectronics devices.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2021
·
IF 8.128
Yanting Tang,Jielin Huang,Shuaifei Liu,Dandan Xiang,Xinqi Ma,Xin Yu,Mingxue Li,Quanhui Guo
Mesocrystals are types of fascinating multifunctional materials in fabricating rapid charge transport pathways, and surface engineering could be considered as a significant influencing factor in boosting charge separation for efficient photocatalytic application. In this work, surface engineered Ta 2 O 5−x mesocrystals were synthesized by facile alkali treatment strategy for enhanced visible light photocatalytic tetracycline degradation. The highly enhanced photocatalytic activity could be attributed to the highly increased surface areas and surface hydroxyl groups to compare with those of commercial Ta 2 O 5 and pristine Ta 2 O 5−x mesocrystals, which could provide more surface reactive sites and high electron density center for trapping photo-generated holes. Besides, possible tetracycline transformation pathways over surface engineered Ta 2 O 5−x mesocrystals and visible light photocatalytic mechanism were also proposed in this work. Current work also provides a facile strategy for regulating surface property of ultrawide bandgaps semiconductors for enhanced visible light photocatalytic performance.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2021
·Vol. 32
·期 14
·19424-19433
·
IF 2.478
Guo Chengbin,Hu Rong,Qiao Hui,Duan Chenguang,Qi Xiang
Titanium dioxide (TiO 2 ) has been widely studied in the field of photocatalysis. However, the development of TiO 2 was limited by the photoresponse only in the ultraviolet region and the rapid recombination of photogenerated electron–hole pairs. In this work, we prepare a novel TiO 2 and two-dimensional (2D) bismuth selenide (Bi 2 Se 3 ) hybrid nanosheets (TiO 2 /Bi 2 Se 3 HNs) via a simple water bath ultrasonic route. X-ray diffraction pattern and Raman spectra were carried out to confirm that as-prepared samples were pure and well crystalized. Besides, TEM characterization proves that 2D Bi 2 Se 3 nanosheets have high specific surface area and it can be clearly observed that the TiO 2 with 60 nm particles are uniformly supported on the surface. Furthermore, photoelectrochemical (PEC) measurements demonstrate that the TiO 2 /Bi 2 Se 3 HNs exhibit excellent photocatalytic performance of 4.3 µA/cm 2 under 100 W of visible light, which were almost 2.5 times that of pure TiO 2 . More importantly, our results show that the photocurrent density was quite stable and only dropped by 10% after 125 cycles. In summary, the improved photocatalytic activity is due to the unique characteristic of 2D Bi 2 Se 3 nanosheets, such as maximized reaction sites and good electrical conductivity, and the positive coupling effect of the TiO 2 /Bi 2 Se 3 heterojunction. These extraordinary properties make the TiO 2 /Bi 2 Se 3 HNs photocatalysts have excellent potential for photocatalytic application.
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JOURNAL OF SOLID STATE CHEMISTRY
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2021
·
IF 3.498
Cong Lu,Weidong Wu,Haifeng Zhou
A novel visible-light-driven BiOBr/BiFeWO 6 heterojunction was prepared through a simple hydrothermal route. The physicochemical properties of BiOBr/BiFeWO 6 nanocomposites were systematically characterized. The existence of a clear interface between BiOBr and BiFeWO 6 could be obtained by transmission electron microscopy , indicating the formation of heterojunction. Rhodamine B (RhB) was used to investigate the photocatalytic performance of BiOBr/BiFeWO 6 nanocomposites under visible light irradiation (λ > 420 nm). The degradation efficiency of BiOBr/BiFeWO 6 -40 nanocomposite reached 96.3 % within 90 min. The improved photocatalytic performance is mainly due to the synergistic interaction between BiOBr/BiFeWO 6 . It is beneficial to the separation of photogenerated carriers and the absorption of visible light. In addition, long-term stability results indicate that BiOBr/BiFeWO 6 heterojunction may be an excellent material for effective degradation of dyes from wastewater and may be explored for large-scale application in the future. Finally, a possible mechanism is proposed for the catalytic degradation of RhB by the BiOBr/BiFeWO 6 heterojunction. This work provides a convenient and dependable method to synthesize BiOBr/BiFeWO 6 nanocomposite, which might be a promising candidate for large-scale application in wastewater treatment.
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