Journal of Cleaner Production
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2023
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IF 11.1
Teng Lu,Zhaomin Li,Liping Du
With declining conventional reserves, tapping heavy oils generates substantial emissions yet is essential to meet energy demands. This study pioneers an integrated approach using silica aerogels to develop thermally stable flue gas foams for enhanced CO 2 sequestration and heavy oil recovery. Microfluidic experiments and molecular dynamics simulations revealed a 5-fold decrease in gas diffusion rates for aerogel-stabilized versus pure surfactant foams at 95 °C due to the ultralow thermal conductivity of the nanoparticle coating layer . The thermally stable nanoengineered foams demonstrated a remarkable 81.23% CO 2 trapping efficiency in heterogeneous cores, surpassing conventional flue gas foam. Additionally, three-dimensional simulations in an oil reservoir model showed improved vertical conformance and oil recovery with aerogel-stabilized foam. The exceptional insulating properties redirected heat downward to enhance sweep efficiency. This novel concept transforms flue gas emissions into value-added foams for concurrent environmental and productivity benefits during heavy oil development.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Wen Wang,Liqiang Qi,Jiahao Zhang
Escaped ammonia emission following Selective Catalytic Reduction denitrification significantly influences subsequent flue gas treatment processes. This study investigates the adsorption capabilities of acid-modified fly ash concerning escaped ammonia (NH 3 ) and its consequential impact on specific resistance. Furthermore, the adsorption mechanism of acid-modified fly ash on NH 3 was explained. Acid activation facilitated the dissolution of a portion of Fe and Al constituents within the fly ash, the contents of Fe and Al in SFA decrease by 4.91% and 5.64%, respectively. In addition, the specific surface area and porosity of fly ash are obviously improved. The specific surface areas of HFA and SFA increased from 1.83 (OFA) to 4.69 and 7.71 m 2 /g, respectively. Adsorption kinetics adhered to the pseudo-first-order model. SFA showed the best adsorption performance, with NH 3 adsorption up to 10.65 mg/g, which was 4.27 times higher than OFA. The creation of a surface liquid film during NH 3 adsorption led to decreased specific resistance values across all fly ash samples after-adsorption. The highest specific resistance values recorded for original fly ash (OFA), hydrochloric acid-modified fly ash (HFA) and sulfuric acid-modified fly ash (SFA) were 6.21 × 10 12 , 3.37 × 10 11 and 5.02 × 10 10 Ω·cm, respectively. Sulfuric acid activation makes fly ash have stronger adsorption capacity for escaping ammonia, and SFA maintains good specific resistance characteristics, which has good application prospects in electrostatic precipitation and air pollution control .
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CARBON
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2023
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IF 10.9
Yuan Li,Jing Gao,Yaxuan Shi,Yazhen Wang,Mengyang Li,Aizhao Pan,Mingyou Hu,Guanjun Zhang
Carbon quantum dots (CQDs) have been widely used in many fields due to their excellent optoelectronic properties. However, the impact of precursor on the structure, properties, and formation mechanism of CQDs under gas-liquid discharge process is poorly understood, which invites more detailed studies toward structure design and fluorescence regulation. In this study, the CQDs of blue fluorescence are successfully synthesized using only low-cost organic solvent such as ethanol, 1-butanol, and 1-hexanol as the precursors by gas-liquid discharges within 5 min. Entering argon gas into the liquid reactant greatly lowers the difficulty of discharges in the liquids and improves the discharge stability, and thereby produce a more uniform particle of the synthesized CQDs. The average size of CQDs synthesized by alcoholic organics is 2–3 nm, and the surfaces of the products are functionalized by various oxygen-containing groups. The CQDs present bright blue fluorescence with an excitation wavelength of 365 nm and exhibit an excitation-dependent property. In situ observations of optical emission spectrometry (OES) during discharges indicate that the precursors are break down into free radicals such as C 2 , CH and H, and then radicals recombine and grow continuously into CQDs. During the formation of CQDs, molecular fluorophores are produced concomitantly. In addition, changing the functional groups of the precursors significantly influences the fluorescence properties of the synthesized CQDs. For CQDs prepared from solvents containing heterogeneous elements such as nitrogen and sulfur show green fluorescence properties, i.e., fluorescence red-shift. This work provides a pathway for fabricating diversified CQDs by modulating the structure and functional groups of the selected precursors.
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Nature Communications
·
2023
·Vol. 14
·期 1
·1-12
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IF 16.6
Guo Luyao,Zhuge Kaixuan,Yan Siyang,Wang Shiyi,Zhao Jia,Wang Saisai,Qiao Panzhe,Liu Jiaxu,Mou Xiaoling,Zhu Hejun,Zhao Ziang,Yan Li,Lin Ronghe,Ding Yunjie
Supported metal clusters comprising of well-tailored low-nuclearity heteroatoms have great potentials in catalysis owing to the maximized exposure of active sites and metal synergy. However, atomically precise design of these architectures is still challenging for the lack of practical approaches. Here, we report a defect-driven nanostructuring strategy through combining defect engineering of nitrogen-doped carbons and sequential metal depositions to prepare a series of Pt and Mo ensembles ranging from single atoms to sub-nanoclusters. When applied in continuous gas-phase decomposition of formic acid, the low-nuclearity ensembles with unique Pt 3 Mo 1 N 3 configuration deliver high-purity hydrogen at full conversion with unexpected high activity of 0.62 mol HCOOH mol Pt −1 s −1 and remarkable stability, significantly outperforming the previously reported catalysts. The remarkable performance is rationalized by a joint operando dual-beam Fourier transformed infrared spectroscopy and density functional theory modeling study, pointing to the Pt-Mo synergy in creating a new reaction path for consecutive HCOOH dissociations.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2023
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IF 9.9
Li Wang,Kun Ge,Jiaqi Duan,Xiaomeng Du,Guoqiang Zhou,Lili Ma,Shutao Gao,Jinchao Zhang
Chemodynamic therapy (CDT) based on hydroxyl radicals (•OH) to suppress tumor cells is a promising strategy due to its efficacy and safety. Nevertheless, in tumor cells, CDT still faces challenges such as insufficient •OH and weak killing effect of tumor cells under physiological conditions due to inadequate amounts of endogenous hydrogen peroxide (H 2 O 2 ) and heightened glutathione expression. These challenges limit the therapeutic potential of CDT. To improve the effects of CDT, combination treatment strategies have been developed. Here, we report a rationally designed nanocomposite (CaO 2 @Cu-LA) with self-supplying H 2 O 2 ability from calcium peroxide, and nitric oxide (NO) generation ability from l -arginine. NO molecules not only exhibit a strong killing effect, but also have the potential to transfer into the more cytotoxic substance peroxynitrite anion by reacting with reactive oxygen species. The results showed that CaO 2 @Cu-LA could significantly suppress tumor growth by increasing •OH radicals and NO molecules. Taken together, the strategy developed here provides a good application foreground to yield a remarkable synergistic antitumor effect of CDT and NO gas therapy.
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SENSORS AND ACTUATORS B-CHEMICAL
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2023
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IF 8.4
Changlin Xiao,Zihuan Tang,Zhuangzhuang Ma,Xiaotong Gao,Hongqiang Wang,Lichao Jia
Metal oxides based semiconductors promise high performance gas sensing owing to their robustness and low cost, but are limited by their unsatisfied adsorption ability and intrinsic low carriers' mobility. We herein demonstrate an efficient strategy of reducing the adsorption energy and improving the carrier mobility via bulk implanted TiO 2 nanocrystals (NCs) in LaFeO 3 porous structure . By implanting laser generated sub-3 nm TiO 2 NCs in LaFeO 3 samples, the response value (221.8 for 100 ppm formaldehyde) increases about 4 times comparing with that of pristine. Additionally, the sample exhibits high sensitivity and fast response/recovery speed toward formaldehyde steam. The detailed analyses and theoretical calculation proves that the TiO 2 NCs could cause the increase of adsorbed oxygen levels as well as the carrier mobility through forming the heterojunction with LaFeO 3 . This work verifies that TiO 2 NCs implanted LaFeO 3 is a promising formaldehyde sensing material, which provides a new approach to improve sensing ability of metal oxide semiconductor (MOS) based gas sensors.
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ENERGY & FUELS
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2023
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IF 5.3
Jianlu Zhu,Youmei Peng,Naiya Xie,Zihe Li,Yixiang Zhang,Wuchang Wang,Yuxing Li
In the process of high expansion foam inhibiting liquefied natural gas (LNG) leakage evaporation, LNG and water in foam will generate hydrates in a normal pressure environment. In order to study the absorption effect of hydrate on LNG vapor, a hydrate formation device in an LNG–foam system was designed. The gas content experiment of hydrate was carried out to evaluate the inhibition effect of hydrate absorption on LNG evaporation, which provides a basis for improving the stability time of hydrate and reducing the escape rate of natural gas. Tetrahydrofuran (THF) will aggravate the foam drainage rupture, thereby weakening the stability of the foam. On the basis of adding a hydrate thermodynamic promoter, nanoparticles were added to enhance the stability of foam. The experimental results show that the foam half-life of 1 wt % THF and 0.5 wt % hydrophilic SiO2 nanoparticles is the longest, which is 1.7 times higher than that without additives. The gas absorption of hydrate formed in the compound system accounts for 57.5% of LNG evaporation gas, which is more than 4 times that without additives.
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JOURNAL OF MEMBRANE SCIENCE
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2021
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IF 8.742
Bo Wang,Jiayou Xu,Jixiao Wang,Song Zhao,Xinlei Liu,Zhi Wang
Gas separation performance of mixed matrix membrane heavily depends on the pore structure of the nanofillers. Metal-organic frameworks (MOFs) are promising platform materials for constructing molecular-selective pores for specific applications. In this work, deliberately-selected polymers with CO 2 affinity (PVAm, Pebax and PEI) are employed as pore regulators to manipulate the pore chemistry and size of MOF UiO-66 nanoparticles and consequently control gas transport rate of CO 2 and N 2 molecules. The branched polymer (polyethyleneimine (PEI)) grafted UiO-66, denoted as UKI, is beneficial to enhancing the membrane selectivity. The UKI doped Pebax/mPSf membranes exhibit CO 2 /N 2 selectivity up to 278, 6.5 times of the bare Pebax/mPSf membranes. Meanwhile, the CO 2 permeance is boosted from around 690 to 1120 GPU (1 GPU = 10 −6 cm 3 (STP)·cm −2 ·s −1 ·cmHg −1 = 3.35 × 10 −10 mol m −2 s −1 ·Pa −1 ). The block copolymer (poly(ether block amide) (Pebax)) grafted UiO-66, denoted as UKX, is conducive to increasing the membrane permeance. The UKX doped Pebax/mPSf membranes exhibited CO 2 permeance up to 1683 GPU, 2.45 times of the bare Pebax/mPSf membranes. Meanwhile, CO 2 /N 2 selectivity increased from around 42 to 146. Additionally, excellent pressure-resistant property and outstanding stability are observed under simulated flue gas .
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2021
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IF 4.539
Zhen Li,Daorong Sun,Jiawen Chi,Songjian Zhao
To enhance mercury removal efficiency at low temperature in flue gas , UiO-66-NH 2 framework was functionalized using halogen group via a diazotization process. -NH 2 was successfully replaced by halogen groups, and diazotization process had little impact on the morphology and the structural information of UiO-66-NH 2 , indicated UiO-66-X (Cl, Br, I) had an excellently chemical stability. Hg 0 capture experiments indicated added iodine (I) functional group was the most effective compared with chlorine (Cl) and bromine (Br). UiO-66-I can reach nearly 100% Hg 0 removal efficiency at 25–150 ℃，and the difference was the duration time for high performance. Moreover, oxygen played an important role for Hg 0 removal, which could be activated by the halogen functional group and then reacted with Hg 0 , finally existed on the adsorbent in the form of UiO-66-X … Hg-O. Furthermore, adsorption kinetic analysis indicated mercury adsorption at surface active sites was the rate controlling step .
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SENSORS AND ACTUATORS B-CHEMICAL
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2021
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IF 7.46
Chen Wang,Yinglin Wang,Pengfei Cheng,Luping Xu,Fan Dang,Tianliang Wang,Zhaohui Lei
A highly sensitive and selective acetone gas sensor has been fabricated successfully by designing n-n heterojunction consisting of TiO 2 nanorods and α -Fe 2 O 3 branches. The structure and morphology of the TiO 2 / α -Fe 2 O 3 nanocomposites were examined via X-ray diffraction and scanning electron microscopy, respectively. TiO 2 nanorod (with the diameter about 42 nm) arrays were in-situ generated on the surface of Al 2 O 3 ceramic tubes by a simple hydrothermal process. In addition, α -Fe 2 O 3 branches grew on TiO 2 stems successfully in the second hydrothermal process. These nanorod branches had a relatively uniform length, which could be tunable by changing the concentration of iron precursor. The gas sensing properties of the pristine and α -Fe 2 O 3 branches-decorated TiO 2 nanorods sensors with regard to acetone gas were investigated. The results indicated that the sensor based on TiO 2 / α -Fe 2 O 3 heterostructures measured at 225 °C had a higher response of 21.9 toward 100 ppm of acetone gas which was about 9 times higher than pristine TiO 2 nanorods sensor. The dominant mechanism for enhanced sensing properties were discussed in detail with the semiconductor depletion layer model and TiO 2 / α -Fe 2 O 3 n–n heterojunction theory.
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ACS Catalysis
·
2021
·
IF 13.084
Li Sun,Junkang Xu,Xiaoyan Liu,Botao Qiao,Lin Li,Yujing Ren,Qiang Wan,Jian Lin,Sen Lin,Xiaodong Wang,Hua Guo,Tao Zhang
Single-atom catalysts (SACs) with complete dispersion of metal species on substrates provide the ultimate atom economy and opportunities for improved heterogenous catalysis or to develop more catalyst formulation. However, atomically dispersed dopants can also improve the catalyst in an indirect capacity. Here, we report an Ir1/α-MoC SAC that exhibits high activity for water gas shift reaction with ∼100% CO conversion at 150 °C. The reaction rate of this catalyst is orders of magnitude higher than previous Ir-based catalysts and ∼4 times that of α-MoC. Experimental characterizations combined with density functional theory (DFT) calculations reveal that such good performance originates from the effective catalysis by the α-MoC substrate with Ir1 serving as a single-atom promoter. DFT calculations also establish a correlation between the active Mo sites and the catalytic performance for water gas shift reaction. This work highlights the possibility of enhancing catalysis by single-atom promoters as a promising strategy for designing effective SACs.
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Inorganic Chemistry Frontiers
·
2021
·Vol. 8
·期 23
·5016-5023
·
IF 6.569
Mengqi Bu,Yang Feng,Qingxun Li,Yiran Wang,Shou Feng,Kai Zhang,Yujie Jiang,Lili Fan,Zixi Kang,Daofeng Sun
Metal–organic framework (MOF) membranes with an ultra-small pore size (<4 Å) have shown great prospects in the highly selective separation of small gas molecules such as hydrogen, but their narrow channels may result in a low gas permeance. To improve the gas permeance of ultra-microporous MOF membranes, a stable covalent organic framework (COF) with large and uniform pores is doped to construct a binary COF/MOF all-nanoporous composite (ANC) membrane, equivalent to reducing the effective membrane thickness but avoiding the challenging ultra-thin membrane preparation. The COF synthesized by ball milling is combined with a metal gel to form a precursor membrane, which was then transformed to a COF/MOF ANC membrane by treatment with the MOF ligand vapor. A very small amount of solvent has been applied, offering an environmentally-friendly preparation process. Compared with the pristine MOF membrane, the COF/MOF ANC membranes possess a highly improved gas permeance from 22 GPU to 551 GPU with a slight sacrifice of selectivity; this introduces a new strategy to optimize the separation performance of MOF membranes.
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