CHINESE JOURNAL OF STRUCTURAL CHEMISTRY
·
2023
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IF 2.2
Qian Liu,Yingyi Wen,Jian-Ze Xiao,Shao-Zhen Luo,Guan-E Wang,Peng-Yi Tang,Xiao-Liang Ye,Gang Xu
The poor sensitivity of metal-oxide (MO) sensing material at room temperature can be enhanced by the modification of noble metal catalysts . However, the large size and uncontrollable morphology of metal nanoparticles (NPs) compromise the catalytic activity and selectivity. Downsizing metal NPs to the atomic level is a promising solution because it offers high activity and selectivity. Nevertheless, a facile and universal approach for stable loading atomic-level metal on MO-based sensing materials is still challenging. Herein, we present a strategy to construct synergetic coordination interface for uniform loading of atomic-level metal catalysts on MO-based gas-sensing materials using a difunctional mediator layer. In this work, atomically dispersed Pt catalysts are coordinately anchored on ZnO nanorods (NRs) using polydopamine (PDA) as a mediator. As a result, compared with pristine ZnO NRs, a six-fold enhanced response of 18,489% is achieved toward 100 ppm NO 2 on 0.20 wt%Pt–ZnO@PDA-1.5 nm, and the selectivity is also promoted. Such sensitivity is higher than that of most reported noble metal-modified MO NO 2 -sensing materials. This work provides a simple and general strategy for building highly sensitive and selective gas-sensing materials using atomic-level noble metal catalyst.
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高影响因子
TALANTA
·
2023
·
IF 6.1
Shutong Yang,Yanqiu Chu,Liancheng Gu,Chuan-Fan Ding,Fengyan Wang
Noncovalent ternary complexes between cyclodextrins (CDs), small molecules and alkali earth cations drew growing attention due to their potential application in many chemical and pharmaceutical fields. To date, the main factors affect the formation mechanism of noncovalent ternary complexes in gas phase have not been fully investigated. In this study, ternary complexes of CDs, divalent metal cations and amino acids (AAs) were investigated by electrospray ionization mass spectrometry (ESI-MS), demonstrating the formation of 1:1:1 stoichiometric noncovalent ternary complex of [CD + cation(II)+AA] 2+ in gas phase. The results revealed that only +2 valence cations can form stable ternary complexes in ESI-MS. The ratio of peak intensities for [β-CD + Mg(II)+AA] 2+ to those for [β-CD + Mg(II)] 2+ hydrophobicity of AAs was also determined to discuss the effect of hydrophobicity of AAs. Exceptions exist for Pro, Gly, and Val indicated that other factors such as side-chain structure and rigidity of AAs can also influence the binding strength for ternary complexes. Collision induced dissociations (CID) were performed to further confirm the formation of the β-CD ternary complexes, revealing the binding strength of [CD + Mg(II)+Phe] 2+ decreased in the order of γ-CD, β-CD, and α-CD. Although Leu and Ile are isomers, the ESI-MS demonstrated the peak intensity for ternary complexe of [β-CD + Mg(II)+Ile] 2+ exhibited stronger than that of [β-CD + Mg(II)+Leu] 2+ , DFT theoretical calculations were conducted to explain the phenomenon. The calculation indicated when Mg 2+ existing, the conformations of the two ternary complexes could be affected due to the electrostatic force . In the complexes, the Leu and Ile turn a way round, inserting to the cavity with their carboxylic acid side into the large rim side of β-CD and interacting with Mg 2+ . This work not only clearly explained the factors influencing the formation of [CD + cation(II)+AA] 2+ in gas phase, but it also provides an insight in designing ternary complexes for areas such as drug design and chiral discrimination.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Mengge Shang,Xiaoqian Peng,Jing Zhang,Xiaochan Liu,Zhipeng Yuan,Xinfu Zhao,Sijia Liu,Shimo Yu,Xibin Yi,Serguei Filatov
Adsorption natural gas (ANG) is a technology in which natural gas is stored on the surface of porous materials at relatively low pressures, which are promising candidates for adsorption of natural gas. Adsorbent materials with a large surface area and porous structure plays a significant role in the ANG technology, which holds promise in increasing the storage density for natural gas while decreasing the operating pressure. Here, we demonstrate a facile synthetic method for rational construction of a sodium alginate (SA)/ZIF-8 composite carbon aerogel (AZSCA) by incorporating ZIF-8 particles into SA aerogel through a directional freeze-drying method followed by the carbonization process. The structure characterization shows that AZSCA has a hierarchical porous structure, in which the micropores originated from MOF while the mesopores are derived from the three-dimensional network of the aerogel. The experimental results show that AZSCA achieved high methane adsorption of 181 cm3·g–1 at 65 bar and 298 K, along with higher isosteric heat of adsorption (Qst) throughout the adsorption range. Thus, the combination of MOF powders with aerogel can find potential applications in other gas adsorption.
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APPLIED CLAY SCIENCE
·
2023
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IF 5.6
Yao Xiao,Zhenchun Xu,Chuansheng Wang,Huiguang Bian
In order to realize the high value-added utilization of natural clay materials in natural rubber composites , an environment-friendly animal glycerol potassium salt was introduced to modify kaolin, and the natural rubber with excellent performance were prepared by high-energy ball milling combined with gas-phase spray drying technology . The impact of the ball milling reduced the particle size and increased the specific surface area of kaolin, promoting the chemical modification of kaolin by potassium oleate. The gas-phase spray technology effectively broke the filler aggregates, and the high-temperature roller realized the instantaneous drying, reducing the oxidation and fracture of the rubber molecular chains . In this paper, the gas barrier properties , mechanical properties, anti-aging properties, dynamic mechanical properties and Payne effect of the composites were investigated. The FTIR , XPS and interfacial contact angle demonstrated the existence of a stable chemical bonding in the process of potassium oleate-modified kaolin, and the hydrophilicity of kaolin was reduced. Kaolin was uniformly and finely dispersed in the rubber matrix by spray drying technology. Compared with the traditional dry mixing, the composites prepared by the technology improved the gas barrier properties , processing properties, comprehensive mechanical properties, and the aging coefficient increased by 23.1%, and had excellent wet skid resistance and rolling resistance.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lu Jia,Yuzhu Wang,Tingting Hu,Chunyu Yang,Huiming Lin,Feng Zhang,Fengyu Qu,Liru Cui,Wei Guo
Photothermal therapy (PTT) has attracted considerable attention in the field of nanomedicine owing to its high efficiency, low invasiveness , and precise controllability. However, limited by the activation of the immune system by PTT and the low penetrating ability of near-infrared lasers, the use of a single PTT is usually ineffective. Herein, a unique injectable hydrogel system was strategically designed and fabricated using CoSnS x , L-arginine, chitosan (CTS), and carboxymethyl cellulose (CMC) for sonodynamic and dual-gas therapy cooperative PTT. CoSnS x with a hollow structure can not only produce a large amount of singlet oxygen ( 1 O 2 ) under ultrasonic (US) irradiation, but also produce H 2 S gas in an acidic environment, so as to achieve sonodynamic and gas therapeutic effects. Additionally, CoSnS x exhibited excellent photothermal conversion efficiency of 48.24% under 808 nm laser irradiation. As a precursor of NO, L-arginine is incorporated into the hydrogel to enable the controlled release of NO under US/laser irradiation, thereby enhancing the PTT effect. Such a multifunctional injectable hydrogel system can achieve high therapeutic efficacy through sonodynamic and dual-gas treatment-enhanced PTT, as demonstrated by both in vitro and in vivo experiments. Our designed injectable hydrogel system provides a unique solution for enhancing the PTT.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junxiong Zhao,Huirui Li,Ruzhen Zhao,Chuang Lei,Qifeng Wei,Xiulian Ren
Using chlorine-containing oxidants to remove pollutants in the exhaust gas of ships is normally accompanied by Cl 2 escape, which poses a significant threat to the environment and the health of the crew. This paper proposes a method to solve the problem of Cl 2 escape in a single NaClO solution system using BAD (a new amide absorbent, C 12 H 25 NO). The electrostatic potential (ESP) theoretical calculations, FT-IR and UV–vis spectra tests showed that the strong field effect interaction between BAD and Cl 2 , which can form a stable symmetrical structure similar to a “sandwich”, results in a strong binding ability of BAD to Cl 2 . The effects of the initial pH, the concentration of NaClO solution, aeration time, and some operating parameters on the loss of active chlorine (AC) components were studied. Under the same conditions, a two-phase composite absorbent system with the addition of BAD can reduce the loss of AC components by 32.67% on average and up to 56.12%. It also can effectively capture the Cl 2 escaping with the gas flow and keep it in the system, which enhances the oxidation of NO by Cl 2 at the gas–liquid interface. It also has a strong ability to remove pollutants for a long period, as the removal efficiencies of SO 2 , NO, and NOx within 20 mins were 97.84%, 77.98%, and 76.01%, respectively. The results show that the BAD-NaClO two-phase composite absorbent system can effectively reduce Cl 2 escape, and it is a sustainable wet treatment scheme for ship exhaust gas with great application prospects.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jia'nan Wang,Wenjun Huang,Haomiao Xu,Peng Cui,Zan Qu,Naiqiang Yan
Sulfur dioxide (SO 2 ), as a primary pollutant in the air, has attracted much attention due to the adverse effects on the atmospheric environment and human health. The wet flue gas desulfurization (WFGD) has been proved to be the most effective method to control the emission of SO 2 . However, the traditional absorbents in WFGD posed the problems of limited recycling utilization and susceptible to oxidation. In this study, we proposed the Na-Mg-Ci 3- compound system to repeatedly absorb SO 2 for rounds. The results demonstrated that the compound system can integrate the absorption capacity of Na 3 Ci absorbent and the regeneration efficiency of Mg 3 Ci 2 absorbent. We compared the performances of the compound systems with different alkaline earth metals (Li, Na, K), and the sodium was most suitable for the circulating desulfurization with the consideration of performance and economy. After that, we investigated the influence of ingredient proportions on the absorbent performance, and the results showed that the 0.4 mol/L Na 3 Ci and 0.2 mol/L Mg 3 Ci 2 were the best combination for the compound system in these experiments. In this condition, the compound system had the excellent effective sulfur capacity and regeneration speed in the recycling process. Moreover, the anti-oxidation effect of sodium ascorbate was explored, and the reusability performance of compound system can be improved with antioxidants. This study contributes to providing a novel method for the removal and recycling of SO 2 in the wet flue gas desulphurization.
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ANALYTICAL CHEMISTRY
·
2023
·
IF 7.4
Peiru Luo,Mengke Bai,Qingyun He,Zifang Peng,Lingyun Wang,Chuan Dong,Zenghua Qi,Wenfen Zhang,Yanhao Zhang,Zongwei Cai
The broad application of plastic products has resulted in a considerable release of microplastics (MPs) into the ecosystem. While MPs in other environmental matrices (e.g., soil and water) have been studied for a long time, the atmospheric fine particulate matter (PM2.5)-bound MPs are rarely investigated due to the lack of an appropriate analytical approach. The prevalently used visual and spectroscopic means (e.g., optical microscopy, Fourier-transform infrared spectroscopy, and Raman spectroscopy) suffer from obvious drawbacks that cannot precisely detect MPs of tiny sizes and provide quantitative information. In the present study, a novel strategy that does not require sample pretreatment was developed to first effectuate accurate quantification of polyethylene MP (PE-MP) in PM2.5 based on pyrolysis-gas chromatography–tandem mass spectrometry (Pyr-GC-MS/MS). It featured acceptable recoveries (97%–110%), high sensitivity (LOD = 1 pg), and qualified precisions (RSD of 3%–13%). Employing this approach, for the first time, exact atmospheric concentrations of PE-MPs in PM2.5 from megacities in North (Zhengzhou and Taiyuan) and South (Guangzhou) China were obtained, and relatively serious pollution was found in Taiyuan. The 100% sample detection rates also suggested the widespread occurrence and possible human exposure risks of PM2.5-bound PE-MPs. In brief, the new strategy could conduct direct, sensitive, and accurate quantification of PE-MP in PM2.5, favoring further studies of environmental fates, distributions, and toxicities of atmospheric MPs.
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MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Yanshuxian Liu,Yilei Fan,Yin Zheng,Zhongping Huang,Huijun Liu,Zhenlu Shen,Yu Xu,Danxia Yu,Xuedong Xiao
A sensitive and novel method for the determination of methamphetamine (MAMP), 3,4-methylenedioxymethamphetamine (MDMA) and their metabolites amphetamine (AMP), 3,4-methylenedioxyamphetamine (MDA) in human hair was established by the employment of flash evaporation-gas chromatography/mass spectrometry (FE-GC/MS) combined with micro-reaction device. 0.30 mg human hair after cutting was put into a sealed glass capillary and heated at 270 °C in a pyrolyzer for 0.5 min. MAMP, AMP, MDMA and MDA evaporated from the hair were converted into their corresponding trifluoroacetylation product in a 60 °C water bath for 30 min with the acetylation by 2 μL trifluoroacetic anhydride (TFAH). Thus, amphetamines (AMPs) in human hair were separated and detected by GC/MS in SIM mode. The obtained calibration curves showed good linearity with the concentrations of MAMP, MDMA and MDA at 1–100 ng/mg, and AMP at 2–100 ng/mg. The linear correlation coefficients (r) were all larger than 0.996. Limits of detection for MAMP, AMP, MDMA and MDA were 0.67, 0.07, 0.17 and 0.07 ng/mg respectively. Limits of quantification for MAMP, AMP, MDMA and MDA were 2.00, 0.20, 0.50 and 0.20 ng/mg respectively. The precision over a range of 0.63–9.98 % were obtained with the recoveries of 92.7–115.2 % for AMPs. Five positive hair samples, three suspicious hair samples and two negative hair samples were successfully analyzed. The results of FE-GC/MS with micro-reaction device were comparable with those found by the referenced method. It was demonstrated that the developed method had potential applications for the analysis of AMPs in hair.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jiali Fu,Pu Huang,Yafei Guo,Kaizhuo Fan,Zixuan Wang,Xinlei Xie,Jun Yu,Chuanwen Zhao
Integrating calcium-looping cycle (CaL) with reverse-water–gas-shift (RWGS) reaction represents an effective path to realizing integrated CO 2 capture and utilization (ICCU). Screening a suitable catalyst to construct highly efficient CaO-based dual function materials (DFMs) is essential for CaL-RWGS. In the current work, M@CaO (M = Ni, Co, Mn, and Fe) DFMs are prepared for CaL-RWGS, and the influence of catalyst component on the structure, CO 2 capture and RWGS performance, and kinetic behaviors of the CaO-based DFMs is investigated. Results show that the interaction between CaO and catalyst affects the average grain size and dispersion of metallic catalyst, oxygen vacancy concentration, surface basicity, and reducibility of CaO-based DFMs. The desired Mn@CaO DFMs exhibit outstanding CaL-RWGS performance at 650 °C, 15%CO 2 and 50%H 2 , with a great CO 2 uptake (12.30 mmol CO 2 /g), a favorable CO yield (5.92 mmol CO/g), and an impressive CO 2 conversion (53.53%), as well as a high CO selectivity (89.98%). Furthermore, Mn@CaO exhibits excellent carbonation and regeneration kinetics but inferior working stability for CO 2 capture and CO production in multiple CaL-RWGS cycles. Overall, Mn could be a competitive and cost-effective catalyst candidate for high-performance CaO-based DFMs for CaL-RWGS applications, while further work is needed to improve cyclic stability.
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SENSORS AND ACTUATORS B-CHEMICAL
·
2023
·
IF 8.4
Haineng Bai,Cheng Feng,Hui Guo,Xiaoli Li,Weifeng Liu,Yamin Feng,Kuili Liu,Dunjun Chen,Youdou Zheng,Fuqiang Guo
Monitoring and reducing NO 2 pollution at room temperature is indispensable for human survival. Thus, we propose a light-activated route (UV light, 100 mW/cm 2 ) to realize a high-performance NO 2 detection based on CuO/rGO gas sensor. The CuO/rGO sensor under UV light illumination exhibits a high response of 22.18–100 ppm NO 2 at 23 ℃, which is approximately 1.36 times of the CuO/rGO sensor and 2.31 times of the CuO sensor under dark, respectively. Meanwhile, under UV light illumination, the CuO/rGO sensor has a fast response/recovery speed of 10.9/30.9 s to 20 ppm NO 2 at 23 ℃, which is obviously better than that under dark. Moreover, the light-activated CuO/rGO sensor has excellent repeatability, selectivity, ultra-low detection limit (50 ppb) and long-term stability. The significantly appealing gas-sensing performance of CuO/rGO sensor is mainly ascribed to the mesoporous structure, high specific surface area and plentiful oxygen vacancy of CuO/rGO nanocomposites . More attractively, the photo-generated carriers and formed heterojunction also greatly improve the carrier migration in the context of the NO 2 /CuO/rGO interaction, enhancing the gas-sensing performance of gas sensor. Our work will provide insight in utilizing light illumination to realize ultrasensitive and room-temperature detection of ppb-level NO 2 gas.
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Chemistry-An Asian Journal
·
2023
·Vol. 18
·期 17
·e202300505
·
IF 4.1
Siqi Li,Yuan Qu,Xiang Lu,Feiyu Zhang,Song Liu,Bin Li
Graphical This work successfully prepared vascular bundle Zn 2 SnO 4 using sorghum straw as a biological template through a simple hydrothermal pathway. The material displays a good gas sensing performance and far exceeds that of untreated materials. This low-cost, efficient, and renewable natural biomass template method has been proven to be an effective strategy for producing high-performance gas-sensing materials. The development of butyl acetate sensors with high sensitivity and selectivity has been highly desirable for its harmful effects on human health. In this work, we developed a high-performance butyl acetate sensor based on vascular bundle structure Zn 2 SnO 4 nanomaterial derived from maize straw. The vascular bundle structure Zn 2 SnO 4 with higher specific surface area obtained by calcination to remove the maize straw template, plays the dual role of accelerating the diffusion of gas molecules and providing more active sites. Our research showed that the sensor had a response of 18 to 100 ppm butyl acetate at a working temperature of 250 °C, with a fast response recovery rate (18 s/25 s), which showed significant improvement compared to the Zn 2 SnO 4 sensor prepared without templates. The improved performance can be attributed to the cross-linked nanoparticle chains and gas collision mechanism of the sensor. These findings highlight the potential of our sensor for the detection of butyl acetate gas.
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