Frontiers in Bioengineering and Biotechnology
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2022
·
IF 6.064
Fu Dongmei,Xie Dazhi,Wang Fei,Chen Bin,Wang Zhen,Peng Fei
T cell activation is vital for immune response initiation and modulation. Except for the strength of the interaction between T cell receptors (TCR) and peptides on major histocompatibility complex molecules (MHC), mechanical force, mediated by professional mechanosensitive ion channels, contributes to activating T cells. The intrinsic characteristic of synthetic micro/nanomotors that convert diverse energy sources into physical movement and force, opening up new possibilities for T cell regulation. In this work, Pd/Au nanomotors with spiky morphology were fabricated, and in the presence of low concentrations of hydrogen peroxide fuel, the motors exhibited continuous locomotion in the cellular biological environment. Physical cues (force and pressure) generated by the dynamic performance are sensed by mechanosensitive ion channels of T cells and trigger Ca2+ influx and subsequent activation. The successful demonstration that mechanical signals generated in the bio microenvironment can potentiate T cells activation, represents a potential approach for cell-based cancer immunotherapy.
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ACS Nano
·
2022
·
IF 18.027
Ting Wang,Liang Chen,Cong Chen,Mengtian Huang,Youju Huang,Shoujie Liu,Benxia Li
Photocatalytic CO2 conversion into a high-value-added C2 product is a highly challenging task because of insufficient electron deliverability and sluggish C–C coupling kinetics. Engineering catalytic interfaces in photocatalysts provides a promising approach to manipulate photoinduced charge carriers and create multiple catalytic sites for boosting the generation of C2 product from CO2 reduction. Herein, a Cuδ+/CeO2-TiO2 photocatalyst that contains atomically dispersed Cuδ+ sites anchored on the CeO2-TiO2 heterostructures consisting of highly dispersed CeO2 nanoparticles on porous TiO2 is designedly constructed by the pyrolytic transformation of a Cu2+-Ce3+/MIL-125-NH2 precursor. In the designed photocatalyst, TiO2 acts as a light-harvesting material for generating electron–hole pairs that are efficiently separated by CeO2-TiO2 interfaces, and the Cu–Ce dual active sites synergistically facilitate the generation and dimerization of *CO intermediates, thus lowering the energy barrier of C–C coupling. As a consequence, the Cuδ+/CeO2-TiO2 photocatalyst exhibits a production rate of 4.51 μmol–1·gcat–1·h–1 and 73.9% selectivity in terms of electron utilization for CO2 to C2H4 conversion under simulated sunlight, with H2O as hydrogen source and hole scavenger. The photocatalytic mechanism is revealed by operando spectroscopic methods as well as theoretical calculations. This study displays the rational construction of heterogeneous photocatalysts for boosting CO2 conversion and emphasizes the synergistic effect of multiple active sites in enhancing the selectivity of C2 product.
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Photonics Research
·
2022
·Vol. 10
·期 3
·628-636
·
IF 7.254
Qian Xiong,Qian Xiong,Qian Xiong,Qian Xiong,Sihao Huang,Zijun Zhan,Juan Du,Juan Du,Juan Du,Juan Du,Xiaosheng Tang,Xiaosheng Tang,Zhiping Hu,Zhengzheng Liu,Zeyu Zhang,Weiwei Chen,Yuxin Leng,Yuxin Leng,Yuxin Leng,Yuxin Leng
In recent years, all-inorganic halide perovskite quantum dots (QDs) have drawn attention as promising candidates for photodetectors, light-emitting diodes, and lasing applications. However, the sensitivity and instability of perovskite to moisture and heat seriously restrict their practical application to optoelectronic devices. Recently, a facile ligand-engineering strategy to suppress aggregation by replacing traditional long ligands oleylamine (OAm) during the hot injection process has been reported. Here, we further explore its thermal stability and the evolution of photoluminescence quantum yield (PLQY) under ambient environment. The modified CsPbBr3 QDs film can maintain 33% of initial PL intensity, but only 17% is retained in the case of unmodified QDs after 10 h continuous heating. Further, the obtained QDs with higher initial PLQY (91.8%) can maintain PLQY to 39.9% after being continuously exposed in air for 100 days, while the PLQY of original QDs is reduced to 5.5%. Furthermore, after adhering CsPbBr3 QDs on the surface of a micro SiO2 sphere, we successfully achieve the highly-efficient upconversion random laser. In comparison with the unmodified CsPbBr3 QDs, the laser from the modified CsPbBr3 QDs presents a decreased threshold of 79.81 μJ/cm2 and higher quality factor (Q) of 1312. This work may not only provide a facile strategy to synthesize CsPbBr3 QDs with excellent photochemical properties but also a bright prospect for high-performance random lasers.
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CHEMICAL ENGINEERING JOURNAL
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2022
·
IF 16.744
Yihui Wang,Wen Guo,Zizheng Zhu,Kai Xu,Hongyan Zhang,Wenxian Wei,Xin Xiao,Wenjie Liang,Maoshuai He,Tingting Yu,Dongen Zhang,Hong Zhao,Xingyou Xu,Tao Yang
The research of active and efficient electrocatalysts is of great importance for the practical application of some energy conversion devices. Improving the catalytic activity and utilization efficiency of noble metal is of great importance for the practical application. Here, we report a one-pot synthesis of porous rhodium octahedra through a corner-induced-selective-deposition (CISD) process. After simple interfacial boron modification, the performances towards oxygen evolution reaction (OER), hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR) in alkaline media were greatly enhanced. Especially, a small overpotential of 31 mV at 10 mA/cm 2 was achieved for HER, and a high half-wave potential of 914 mV was obtained for ORR, much better than the commercial Pt/C catalysts (55 mV, 891 mV). Density functional theory (DFT) calculation reveals that the boron incorporation optimizes the adsorption properties of catalyst surface and in turn, lowers the overpotentials for the three reactions. This work may be extended to design other nanoscale functional materials with delicate nanostructures and optimized compositions.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2022
·
IF 6.371
Yantong Lu,Shaofan Fang,Guangshe Li,Liping Li
Low-dimensional copper (I)-based ternary metal halides , having the features of nontoxicity, outstanding optical performance and great air-stability, is becoming the promising substitutes for traditional metal perovskite halides . Despite the impressive progress in copper halides, highly effective synthesis of their nanocrystals with precise shape and size control, compared to that of conventional lead halide semiconductors, is still remained to be explored. In this work, we report a systematically optimized finds for the colloidal synthesis conditions of Cs 3 Cu 2 Cl 5 nanocrystals (NCs). The Cs 3 Cu 2 Cl 5 NCs are modulated from nanoparticles to nanorods and to nanoplates by adjusting reaction temperature and reaction time. Cs 3 Cu 2 Cl 5 nanorods give a wide emission at 510 nm, being caused by self-trapped exciton state with exciton binding energy of 137 meV and phonon–electron interaction of 25 meV as determined by temperature-dependent photoluminescence spectra. The photoluminescence quantum yield (PLQY) of the nanorods that were reacted at 150 °C for 1200 s, an optimal reaction condition, reaches up to 80.19%. We also find for the first time that the optical quality of Cs 3 Cu 2 Cl 5 NCs is positively related to the full width at half maximum of main peak in X-ray diffraction pattern . The findings in this work give a view to the future planning for Cs 3 Cu 2 Cl 5 ’s colloidal synthesis and raise an intuitive criterion for the quality of as-synthesized Cs 3 Cu 2 Cl 5 NCs.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Zhichong Shi,Donglei Zhou,Yanjie Wu,Gencai Pan,Wen Xu,Nan Wang,Shuainan Liu,Rui Sun,Le Liu,Xinmeng Zhuang,Yuhong Zhang,Siyu Lu,Hongwei Song
The light loss caused by the incomplete utilization of the solar energy spectrum is a key factor that impedes the photoelectric conversion efficiency of perovskite solar cells (PSCs). Hence, reducing the light escape through enhancing the utilization of ultraviolet (UV) light, and expanding the response of PSCs in the near-infrared (NIR) range is the key factor to further improve the photoelectric conversion efficiency (PCE) of PSCs. However, there is a lack of literature on engineering UV and NIR light harvesting at the same time. Herein, the NaYF 4 :Ce,Tb@NaYF 4 core–shell nanocrystals with efficient photon downconversion ability from UV to visible are designed to be embedded in the electron transporting layer (ETL), which serves as the photon downconverters and defect passivators, successfully improving the light response in both UV and visible region. The CIGSe quantum dots (QDs) with excellent infrared light harvesting ability, together with the plasmonic Au nanorods (NRs), are assembled in the hole transporting layer (HTL) to expand and improve the NIR light harvesting. The light response of the PSCs was successfully broadened to the NIR region from 800 to 920 nm. As a result, the champion PSC device insulating with NaYF 4 :Ce,Tb@NaYF 4 nanocrystals and CIGSe QDs demonstrates a remarkably increased PCE from 19.38% to 22.60%. The modified PSC devices also demonstrate highly improved UV and long-term stability. This work suggests a universal strategy to improve the UV and near-infrared light harvesting of PSCs, which is of great importance for fabricating PSCs with response to full spectrum.
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Biosensors-Basel
·
2022
·Vol. 12
·期 2
·52
·
IF 5.743
Jing Neng,Caiping Liao,Yazhi Wang,Yan Wang,Kai Yang
Molecularly imprinted polymers (MIPs) specifically targeting pentachloronitrobenzene (PCNB) and containing silver nanoparticles have been prepared by free radical polymerization reaction using methyl methacrylate (MMA) as a functional monomer, PCNB as a template molecule, 1,4-butanedioldimethacrylate as a cross linker, lauroyl peroxide (LPO) as an initiator, and the silver nanoparticles with the best surface-enhanced Raman scattering (SERS) effect as SERS enhancement materials. Our results indicated that MIPs specifically recognize PCNB from complex matrices. The intensity of the PCNB characteristic peak was proportional to the concentration, with a linear range of 0.005 to 0.15 μg/mL and a limit of detection of 5.0 ng/mL. The recovery rates and relative standard deviation for the detection of PCNB spiked in the rice samples were from 94.4% to 103.3% and from 4.6% to 7.4%, respectively. The experimental results are consistent with those by the GC-MS method, indicating that the rapid detection of PCNB in food matrices by SERS-MIPs is reliable. In view of the insolubility of PCNB in water, oil-soluble silver nanoparticles were synthesized which can be expanded to detect oil-soluble toxic substances. For the first time, the proposed method provides a point-of-care and cost-effective tool for rapidly detecting PCNB in food matrices with high sensitivity and selectivity by employing SERS-MIPs method.Keywords:surface-enhanced Raman spectroscopy;molecularly imprinted polymers;detection;pentachloronitrobenzene;oil-soluble silver nanoparticles;pesticide residues
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Liya Cao,Shuangshuang Shi,Fangfang Li,Zhongzhi Tian,Shu Xu,Chong Geng
Formation of organometal lead halide perovskite nanocrystals (OPNCs) occurs in fast time scales from milliseconds to seconds, thus posing a hurdle to the growth kinetic study of OPNCs. Water-oil interfacial reaction provides an effective approach for retarding the growth of CH 3 NH 3 PbBr 3 OPNCs. Herein, we investigate systematically the kinetics of CH 3 NH 3 PbBr 3 NCs in water–oil reaction by in situ optical characterization, and identify the key factors governing the growth of OPNCs. Molecular polarity and viscosity of the solvent are found to be crucial to the diffusion step by affecting the diffusion coefficient of CH 3 NH 3 + . Covalent characteristic of the Pb source and molecular structure of the ligands have an impact on the rate-limiting step of PbBr 6 4- formation. In addition, we establish the reaction condition that enables controlled growth of formamidinium lead bromide NCs, thereby demonstrating the application of the growth kinetic in the synthesis of other OPNCs. Kinetic investigation of OPNCs provides a better understanding of their crystallization process that helps guide the development of quantum confined OPNCs for optoelectronic applications.
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LANGMUIR
·
2022
·
IF 4.331
Jian Wang,Jiwen Si,Yizhan Hao,Jingyao Li,Peiping Zhang,Chuanxiao Zuo,Bo Jin,Yan Wang,Wei Zhang,Wenqing Li,Ruifeng Guo,Shiding Miao
Halloysite-based tubular nanorockets with chemical-/light-controlled self-propulsion and on-demand acceleration in velocity are reported. The nanorockets are fabricated by modifying halloysite nanotubes with nanoparticles of silver (Ag) and light-responsive α-Fe2O3 to prepare a composite of Ag–Fe2O3/HNTs. Compared to the traditional fabrication of tubular micro-/nanomotors, this strategy has merits in employing natural clay as substrates of an asymmetric tubular structure, of abundance, and of no complex instruments required. The velocity of self-propelled Ag–Fe2O3/HNTs nanorockets in fuel (3.0% H2O2) was ca. 1.7 times higher under the irradiation of visible light than that in darkness. Such light-enhanced propulsion can be wirelessly modulated by adjusting light intensity and H2O2 concentration. The highly repeatable and controlled “weak/strong” propulsion can be implemented by turning a light on and off. With the synergistic coupling of the photocatalysis of the Ag–Fe2O3 heterostructure and advanced oxidation in H2O2/visible light conditions, the Ag–Fe2O3/HNTs nanorockets achieve an enhanced performance of wastewater remediation. A test was done by the catalytic degradation of tetracycline hydrochloride. The light-enhanced propulsion is demonstrated to accelerate the degradation kinetics dramatically. All of these results illustrated that such motors can achieve efficient water remediation and open a new path for the photodegradation of organic pollutions.
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Frontiers in Chemistry
·
2022
·
IF 5.545
Wang Qian,Gao Long,Yu Chenxi,Wang Meng,Gou Lijie,Zhang Jiaqi
Ligands on the surface of perovskite nanocrystals are important to stabilize the nanocrystal structure. However, the research of ligands on Mn2+ ion-doped CsPbCl3 nanocrystals (Mn: CsPbCl3 NCs), a promising candidate family for the lightning community, is relatively rare. Here, we demonstrate a new ligand modification strategy for preparing high-quality Mn: CsPbCl3 NCs by a simple hot-injection method. Thiophene derivative, for the first time, is applied as ligands for perovskite nanocrystals. The new ligands of thiophene derivatives passivate defects on the surface of NCs and enhance optical properties, originating from the sulfur in thiophene additives binding to the uncoordinated lead ions. The photoluminescence quantum yield of the modified Mn: CsPbCl3 NCs is 93% in comparison with 46% of the pristine counterparts, whose value is the highest to date for ligand-modified Mn: CsPbCl3 NCs. Meanwhile, the thermal, storage, and purification stability are also significantly improved. The performance of related LEDs is also investigated.
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NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 14
·6461-6469
·
IF 3.925
Li'an Peng,Yongxiao Tuo,Yan Lin,Cuiping Jia,Shutao Wang,Yan Zhou,Jun Zhang
Nickel sulfide (NiS) has sparked considerable interest as a promising electrode material for supercapacitors. However, the poor electrical conductivity and unstable structure during the continuous charge–discharge process have limited its practical applications to a great extent. Herein, we report a two-step solvent-thermal method to synthesize phosphorus-doped NiS nanocrystals (P-NiS). The bulk doping of P not only enhances the electrical conductivity and increases the number of electrochemical active sites, but also strengthens the structural stability of the NiS nanomaterial. As a result, the synthesized P-NiS demonstrated an impressive electrochemical performance with a high specific capacity (727.79 C g−1), superior rate performance (50.60% capacity retention at 50 A g−1), and excellent cycling stability (93.10% capacity retention after 3000 cycles). Furthermore, a hybrid supercapacitor (HSC) of P-NiS//AC was assembled in a 2 M KOH electrolyte. It delivered a maximum energy density of 39.80 W h g−1 at the power density of 809.50 W kg−1 and cycling stability with 89.70% capacity retention after 6000 cycles at 1.6 V. This study provided an effective strategy to achieve the bulk doping of heteroatoms into the transition metal sulfides for improving the intrinsic properties of electrodes in electrochemical energy-storage devices.
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ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Yanli Zhu,Jikai Wang,Haitao Xie,Hailing Liu,Shuangquan Liu,Dongxiu He,Pengbing Mi,Suisui He,Jun Wang,Yiyang Sun
Sub-10 nm monodisperse alkaline-earth sulfide nanodots (ASNDs) with bright near-infrared (NIR)-excitation fluorescence and adjustable emission wavelength were prepared by a thermal decomposition method for the first time. The ASNDs exhibited high NIR-to-vis conversion efficiency and served as multicolor fluorescent labels in the proposed miR-224 assay. Targeted detection of the miR-224 level and single-nucleotide variation in miR-224 was carried out on a smartphone-based platform using a hybridization chain reaction (HCR) amplification strategy. In the presence of miR-224, the ASND-labeled HCR probes self-assembled on the surface of the diagnosis kits, generating strong fluorescent signals linearly proportional to miR-224 contents in the range of 10–2000 fM. Significantly, mutations in miR-224 led to the variation in the fluorescence intensity ratio in RGB channels. Simultaneously, evident changes of fluorescent brightness and color were easily visualized by the naked eye, which enabled on-site discrimination of miR-224 with different mutant loci. This work provides a novel preparation approach for ultrasmall NIR excitation sulfide nanodots and reveals the potential of the as-synthesized ASNDs in point-of-care (POC) nucleic acid testing. Further, it may provide a handheld platform for miRNA single-nucleotide polymorphism analysis.
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危险品化学品经营许可证（带存储）