Nature Nanotechnology
·
2023
·Vol. 18
·期 3
·299-306
·
IF 38.3
Wei Pengfei,Gao Dunfeng,Liu Tianfu,Li Hefei,Sang Jiaqi,Wang Chao,Cai Rui,Wang Guoxiong,Bao Xinhe
Tuning catalyst microenvironments by electrolytes and organic modifications is effective in improving CO 2 electrolysis performance. An alternative way is to use mixed CO/CO 2 feeds from incomplete industrial combustion of fossil fuels, but its effect on catalyst microenvironments has been poorly understood. Here we investigate CO/CO 2 co-electrolysis over CuO nanosheets in an alkaline membrane electrode assembly electrolyser. With increasing CO pressure in the feed, the major product gradually switches from ethylene to acetate, attributed to the increased CO coverage and local pH. Under optimized conditions, the Faradaic efficiency and partial current density of multicarbon products reach 90.0% and 3.1 A cm −2 , corresponding to a carbon selectivity of 100.0% and yield of 75.0%, outperforming thermocatalytic CO hydrogenation. The scale-up demonstration using an electrolyser stack achieves the highest ethylene formation rate of 457.5 ml min –1 at 150 A and acetate formation rate of 2.97 g min –1 at 250 A.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
·
IF 16.6
Sun FuYao,Liu LongFei,Liu Tong,Wang XueBin,Qi Qi,Hang ZuSheng,Chen Kai,Xu JianHua,Fu JiaJun
Catastrophically mechanical failure of soft self-healing materials is unavoidable due to their inherently poor resistance to crack propagation. Here, with a model system, i.e., soft self-healing polyurea, we present a biomimetic strategy of surpassing trade-off between soft self-healing and high fracture toughness, enabling the conversion of soft and weak into soft yet tough self-healing material. Such an achievement is inspired by vascular smooth muscles, where core-shell structured Galinstan micro-droplets are introduced through molecularly interfacial metal-coordinated assembly, resulting in an increased crack-resistant strain and fracture toughness of 12.2 and 34.9 times without sacrificing softness. The obtained fracture toughness is up to 111.16 ± 8.76 kJ/m 2 , even higher than that of Al and Zn alloys. Moreover, the resultant composite delivers fast self-healing kinetics (1 min) upon local near-infrared irradiation, and possesses ultra-high dielectric constants (~14.57), thus being able to be fabricated into sensitive and self-healing capacitive strain-sensors tolerant towards cracks potentially evolved in service.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 14
·40534-40550
·
IF 5.8
Fang Lei,Wu Guojian,Yao Keyu,Zhang Dongyang,Zhou Yongchao
A novel heterogeneous catalyst named MoS 2 /MIL-53(Fe, Cu) (MMFC) was prepared by hydrothermal method and applied in a heterogeneous electro-Fenton (hetero-EF) system for lomefloxacin (LOM) degradation in this work. Under the optimal conditions of current density 3 mA/cm 2 , catalyst dosage 0.100 g/L, and initial pH 6, 93.5% LOM (2 mg/L) removal efficiency was achieved in the MMFC hetero-EF system within 60 min, indicating an obvious improvement compared with the MIL-53(Fe, Cu) hetero-EF system. The good catalytic activity was attributed to more effective active sites of the catalyst and the conversion of Fe(II)/Fe(III) and Cu(I)/Cu(II) promoted by Mo(IV) in MoS 2 , which could be inferred by scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS) characterizations. The reusability and stability of MMFC were explored based on five cyclic experiments, and the average degradation efficiency reached 73.9%. Furthermore, the hetero-EF system could achieve the total removal of moxifloxacin and tetracycline within 6 min and 40 min, respectively. Quenching experiments revealed that the hydroxyl radicals (·OH) were the main reactive radicals while superoxide radicals (·O 2 − ) and singlet oxygen ( 1 O 2 ) played a certain part in LOM degradation. Finally, the possible mechanism of the hetero-EF process and LOM degradation pathways were proposed, including substitution, elimination, and cleavage of ring structures. Accounting for good catalytic performance, low preparation cost, and satisfactory versatility, the MMFC exhibited good potential to work as a hetero-EF catalyst for wastewater treatment.
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Nature Energy
·
2023
·Vol. 8
·期 3
·294-303
·
IF 56.7
Luo Long,Zeng Haipeng,Wang Zaiwei,Li Min,You Shuai,Chen Bin,Maxwell Aidan,An Qinyou,Cui Lianmeng,Luo Deying,Hu Juntao,Li Shangzhi,Cai Xueqing,Li Weixi,Li Lin,Guo Rui,Huang Rong,Liang Wenxi,Lu Zheng-Hong,Mai Liqiang,Rong Yaoguang,Sargent Edward H.,Li Xiong
Two-dimensional (2D) and quasi-2D modifications of three-dimensional (3D) perovskite active layers have contributed to advances in the performance of perovskite solar cells (PSCs). However, the ionic diffusion between the surface 2D and bulk 3D perovskites leads to the degradation of the 3D/2D perovskite heterostructures and limits the long-term stability of PSCs. Here we incorporate a cross-linked polymer (CLP) on the top of a 3D perovskite layer and then deposit a 2D perovskite layer via a vapour-assisted two-step process to form a 3D/CLP/2D perovskite heterostructure. Photoluminescence spectra and thickness-profiled elemental analysis indicate that the CLP stabilizes the heterostructure by inhibiting the diffusion of cations (formamidinium, FA + and 4-fluorophenylethylammonium, 4F-PEA + ) between the 2D and 3D perovskites. For devices based on carbon electrodes, we report small-area devices with an efficiency of 21.2% and mini-modules with an efficiency of 19.6%. Devices retain 90% of initial performance after 4,390 hours operation under maximum power point tracking and one-sun illumination at elevated temperatures.
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JOURNAL OF MATERIALS SCIENCE-MATERIALS IN ELECTRONICS
·
2023
·Vol. 34
·期 3
·1-15
·
IF 2.8
Jiang Xiangqian,Chen Weiping,Li Ling,Gao Peng,Ban Chuncheng,Hao Jiandong,Shi Ningqiang
Boron Nitride Aerogels/PEDOT: PSS composite film with good thermoelectric properties were prepared by a simple preparation process. Boron nitride aerogels with a width of less than 1 μm and thickness of approximately 15 nm were prepared by a combination of freeze-drying and high-temperature tubular furnace heating. Then, boron nitride aerogels material was impregnated in a certain amount of 3, 4-ethylenedioxythiophene monomer polymer: polystyrene sulfonate (PEDOT: PSS) solution by ultrasonic vibration and magnetic stirring to produce a composite film. The output voltage of the flexible Boron Nitride Aerogels/PEDOT: PSS/Au piezoelectric sensor increases with an increase in the bending angle. When the bending angle is greater than 90°, the output voltage reaches 4.03 V. For the sake of broaden the application prospect of nanocomposite films, flexible wearable thermoelectric devices were prepared. Using the human body as a heat source, the output voltage of flexible thin-film thermoelectric devices can reach 233.6 mV. According to the formula calculation, the Seebeck coefficient is 18.54 mV/K and the thermoelectric power factor is 28.86 μW/mK 2 . With improvements in the energy collection capacity of wearable energy devices, we believe that more work will be done in the future to realize the coordinated development of functionality, comfort and health on the basis of improving energy conversion efficiency.
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Nano-Micro Letters
·
2022
·Vol. 15
·期 1
·1-18
·
IF 23.655
Shi Bori,Wang Pingyang,Feng Jingyun,Xue Chang,Yang Gaojie,Liao Qingwei,Zhang Mengying,Zhang Xingcai,Wen Weijia,Wu Jinbo
The split-ring topography is studied systematically from wettability, evaporation assembly to optoelectronic devices.
An efficient dual-function laser etching scheme has been developed to fabricate the split-ring lyophilic pattern and the lateral electrode array simultaneously.
A non-contact human-machine interface based on CsPbBr 3 perovskite photodetector arrays has been successfully applied to wearable devices, automobile displays, robot remote control.
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Scientific Reports
·
2022
·Vol. 12
·期 1
·1-13
·
IF 4.996
Zhou Bin,Sha Shanshan,Tao Juan,Li Jun,Shen Chen,Zhu Jinjin,Tan Lulu,Dong Liyun,Huang Changzheng
Cutaneous melanoma (CM, hereafter referred to as melanoma) is a highly malignant tumor that typically undergoes early metastasis. Pyroptosis, as a special programmed cell death process that releases inflammatory factors and has been widely studied in tumors, but its role in melanoma has not been fully elucidated. In this study, we examined the relationship between pyroptosis and the prognosis of melanoma through bioinformatic analysis of RNA-sequencing data. Our results demonstrated that pyroptosis is a protective factor associated with melanoma prognosis. A higher pyroptosis score was associated with a more favorable overall survival. We used weighted gene co-expression networks analysis (WGCNA) to establish an effective prognosis model based on 12 pyroptosis-related genes. We then validated it in two independent cohorts. Furthermore, a nomogram combining clinicopathological characteristics and a pyroptosis-related gene signature (PGS) score was designed to effectively evaluate the prognosis of melanoma. Additionally, we analyzed the potential roles of pyroptosis in the tumor immune microenvironment and drug response. Interestingly, we found that the elevated infiltration of multiple immune cells, such as CD4 + T cells, CD8 + T cells, dendritic cells, and M1 macrophages, may be associated with the occurrence of pyroptosis. Pyroptosis was also related to a better response of melanoma to interferon-α, paclitaxel, cisplatin and imatinib. Through Spearman correlation analysis of the 12 pyroptosis-related genes and 135 chemotherapeutic agents in the Genomics of Drug Sensitivity in Cancer database, we identified solute carrier family 31 member 2 ( SLC31A2 ) and collagen type 4 alpha 5 chain ( COL4A5 ) as being associated with resistance to most of these drugs. In conclusion, this PGS is an effective and novelty prognostic indicator in melanoma, and also has an association with the melanoma immune microenvironment and melanoma treatment decision-making.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Liu Heming,Xie Ruikuan,Luo Yuting,Cui Zhicheng,Yu Qiangmin,Gao Zhiqiang,Zhang Zhiyuan,Yang Fengning,Kang Xin,Ge Shiyu,Li Shaohai,Gao Xuefeng,Chai Guoliang,Liu Le,Liu Bilu
Constructing stable electrodes which function over long timescales at large current density is essential for the industrial realization and implementation of water electrolysis. However, rapid gas bubble detachment at large current density usually results in peeling-off of electrocatalysts and performance degradation, especially for long term operations. Here we construct a mechanically-stable, all-metal, and highly active CuMo 6 S 8 /Cu electrode by in-situ reaction between MoS 2 and Cu. The Chevrel phase electrode exhibits strong binding at the electrocatalyst-support interface with weak adhesion at electrocatalyst-bubble interface, in addition to fast hydrogen evolution and charge transfer kinetics. These features facilitate the achievement of large current density of 2500 mA cm −2 at a small overpotential of 334 mV which operate stably at 2500 mA cm −2 for over 100 h. In-situ total internal reflection imaging at micrometer level and mechanical tests disclose the relationships of two interfacial forces and performance of electrocatalysts. This dual interfacial engineering strategy can be extended to construct stable and high-performance electrodes for other gas-involving reactions.
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Journal of Analysis and Testing
·
2022
·Vol. 7
·期 2
·163-171
·
IF 0
Qu Gang,Chen Bo,Liu Shilei,Zhang Qiaoli,Yang Yang,Fu Qingshan
Organophosphate nerve agents (OPNAs) are lethal chemical weapons (CWs) which hydrolyze rapidly to alkyl phosphate compounds in the environment. The identification of alkyl phosphate compounds in the environment is critical for the verification of OPNAs. Currently, due to the complex sample preparation and long detection process for organophosphate nerve agent hydrolysis products (OPNAHPs), their high-throughput determination is difficult. To simplify sample preparation and detection of OPNAHPs from environmental samples, a quick, easy, cheap, effective, rugged and safe (QuEChERS) method for the simultaneous purification of the five OPNAHPs in environmental samples combined with detection through direct analysis in real-time ionization source coupled with tandem mass spectrometer (DART-MS/MS) was developed. An internal standard method was applied for the quantification. The method exhibited a good linearity ( R 2 > 0.991) in the range of 1.00 ng/mL-4.00 μg/mL. The limits of detection and limits of quantification were 1.00–7.00 ng/mL and 10.0–20.0 ng/mL, respectively. The recoveries of OPNAHPs in environmental samples were between 65.3% and 107%, with relative standard deviations ranged from 1.6% to 19%. In addition, the sample preparation and analysis process for OPNAHPs could be completed in less than 10 min. The results demonstrated that the modified QuEChERS method could quickly and efficiently remove the matrix of environmental samples. Combined with DART-MS/MS, an accurate and high-throughput detection method of OPNAHPs in environmental samples was provided. The developed method has great potential in the fields of early warning, clinical treatment and environmental decontamination.
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Nature Communications
·
2022
·Vol. 13
·期 1
·1-14
·
IF 17.694
Zhou Liang,Lei Qi,Guo Jimin,Gao Yuanyuan,Shi Jianjun,Yu Hong,Yin Wenxiang,Cao Jiangfan,Xiao Botao,Andreo Jacopo,Ettlinger Romy,Jeffrey Brinker C.,Wuttke Stefan,Zhu Wei
Deoxyribonucleic acid (DNA) is the blueprint of life, and cost-effective methods for its long-term storage could have many potential benefits to society. Here we present the method of in situ cryosilicification of whole blood cells, which allows long-term preservation of DNA. Importantly, our straightforward approach is inexpensive, reliable, and yields cryosilicified samples that fulfill the essential criteria for safe, long-term DNA preservation, namely robustness against external stressors, such as radical oxygen species or ultraviolet radiation, and long-term stability in humid conditions at elevated temperatures. Our approach could enable the room temperature storage of genomic information in book-size format for more than one thousand years (thermally equivalent), costing only 0.5 $/person. Additionally, our demonstration of 3D-printed DNA banking artefacts, could potentially allow ‘artificial fossilization’.
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RARE METALS
·
2023
·Vol. 42
·期 4
·1261-1273
·
IF 8.8
Li Yang,Tang Ming-Yang,Zhang Zhong-Gang,Li Qi,Li Jing-Lei,Xu Zhuo,Liu Gang,Li Fei
BaTiO 3 ceramics are difficult to withstand high electric fields, so the energy storage density is relatively low, inhabiting their applications for miniaturized and lightweight power electronic devices. To address this issue, we added Sr 0.7 Bi 0.2 TiO 3 (SBT) into BaTiO 3 (BT) to destroy the long-range ferroelectric domains. Ca 2+ was introduced into BT-SBT in the form of CaTiO 3 (CT), which has the effect of inhibiting the movement of A-site defects to reduce dielectric loss and refining the grains to increase the breakdown field strength. In addition, we have increased the density and grain uniformity of ceramics by repeated rolling of the green samples through the viscous polymer processing (VPP), to further increase the breakdown electric field. The BT-SBT-CT ceramics exhibit the high recoverable energy storage density of 4.0 J·cm −3 under electric field of 480 kV·cm −1 . Its recoverable energy storage density varies by less than 8% in the temperature range of 30–150 °C, indicating good temperature stability of the energy storage performance. In this work, the energy storage performance of barium titanate-based ceramics was greatly improved by transforming ferroelectrics into relaxor ferroelectrics and VPP method, which can bring new inspiration for the research of energy storage ceramics. Graphical abstract
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Biomass Conversion and Biorefinery
·
2023
·
IF 4
Wen Yao,Zeng Xiang,Tan Hongyu,Liu Bing
To research the optimization of ultrasonic-assisted extraction of total flavonoids from Cortex Lycii and its biological activities. Box-Behnken design experiment was used to optimize the extraction process, and AB-8 macroporous resin was used for purification. Its biological activities were studied by the inhibition rate of α -glucosidase and α - amylase and the scavenging rate of DPPH and ABTS. The optimal extraction parameters of total flavonoids from Cortex Lycii were as follows: the extraction temperature was 63 ℃, the ethanol volume fraction was 71%, the solid–liquid ratio was 28 mL/g, the extraction time was 61 min. Under this optimal condition, the yield of total flavonoids was 1.674 mg/g, which was consistent with the predicted value of 1.637 mg/g, and was 5.85 times higher than that of the traditional water extraction method. The inhibitory rate (IC 50 ) of total flavonoids extract from Cortex Lycii on α -glucosidase was 3 μg/mL and on α -amylase was 5 μg/mL. The scavenging rate (IC 50 ) of DPPH radical was 0.648 mg/mL and the scavenging rate (IC 50 ) of ABTS radical IC 50 was 0.012 mg/mL. The optimized extraction process with response surface design was reliable, which could be used for the extraction of total flavonoids from Cortex Lycii . It has strong hypoglycemic and antioxidant activities and has a good prospect for future utilization and development.
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