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OBJECTIVES: Voice rest is commonly recommended for patients with benign vocal fold lesions (BVFLs) after phonomicrosurgery. The study compares the clinical voice outcomes of two protocols, 7-day complete voice rest (CVR) and 3-day CVR followed by 4-day relative voice rest (CVR + RVR), for patients with BVFLs after phonomicrosurgery. STUDY DESIGN: Prospective, randomized controlled trial. METHOD: Patients with BVFLs undergoing phonomicrosurgery were recruited prospectively and randomly assigned to either protocol. Outcomes were assessed on objective measures of acoustics (fundamental frequency, frequency range, mean intensity, cepstral peak analysis) and aerodynamics (vital capacity, airflow rate, subglottal pressure, phonation threshold pressure), as well as subjective measures, both provider-reported through the Consensus Auditory-Perceptual Evaluation of Voice (CAPE-V), and patient-reported through the Voice Handicap Index (VHI). Clinical measures were collected at three-time points: preoperatively, 1-week postoperatively (on voice rest), and 1-month postoperatively. In addition, adherence was estimated using a vocal dosimeter. RESULTS: Twenty-five patients were recruited and randomized to 7-day CVR (n = 13) and CVR + RVR regimen (n = 12). Statistically significant changes were found within both groups for subglottal pressure (p = 0.03) and VHI score (p < 0.001) comparing pre-operative baseline to 1-month postoperative follow-up. There were no statistically significant differences between the groups. Regardless of group assignment, a significant decrease in overall severity ratings for the CAPE-V was found by comparing the preoperative scores to postoperative scores at 1-week (p < 0.001) and 1-month (p < 0.001). CONCLUSION: Both groups improved their overall voice quality comparably 1 month after undergoing phonomicrosurgery as measured by objective and subjective parameters. LEVELS OF EVIDENCE: 2. Laryngoscope, 134:2812-2818, 2024.
Sujet(s)
Microchirurgie , Plis vocaux , Qualité de la voix , Humains , Femelle , Mâle , Microchirurgie/méthodes , Études prospectives , Adulte d'âge moyen , Plis vocaux/chirurgie , Plis vocaux/physiopathologie , Adulte , Résultat thérapeutique , Maladies du larynx/chirurgie , Maladies du larynx/physiopathologie , Repos/physiologie , Troubles de la voix/étiologie , Troubles de la voix/chirurgie , Troubles de la voix/physiopathologie , Phonation/physiologie , Sujet âgéRÉSUMÉ
Phenylglyoxalic acid (PGA) is a typical metabolite produced by the invasion of styrene into the human body. The detection of PGA can not only reflect the health status of the human body but also assess the level of styrene contamination in the environment. Herein, a novel Eu(III)-MOF (Eu-ttpd) with excellent fluorescence properties was designed by employing the tetrazole-based ligand of 5-((4'-(tetrazol-5'-yl)benzyl)oxy) isophthalic acid (H2ttpd), which successfully used a fluorescent sensor for PGA. The as-synthesized Eu-ttpd features the unique 10-connected tetranuclear cluster [Eu4(µ3-O)2(COO)8]4+ and exhibits a novel (3,10)-connected topological. Benefiting from the perfectly matched excited-state energy levels of the employed H2ttpd ligand with PGA, rapid photoinduced electron transfer (PET) and Dexter-ET can occur, which entitle Eu-ttpd a fast fluorescence quenching response to PGA with a remarkable LOD of 0.269 µM. More importantly, by integrating Eu-ttpd and Mg,N-CDs into the polyacrylamide hydrogel, we optimized Eu-ttpd into a hydrogel sensor which exhibited enhanced detection ability (LOD = 0.052 µM) accompanied by a distinguished color transformation (red-to-blue) and realized ultrasensitive and visual detection of PGA. This work offers an indication for the development of smart sensing materials for human health and environmental safety.
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Excessive use of pesticides has brought about serious environmental risks worldwide that pose significant harm for human health. Herein, a series of metal-organic framework (MOF)-based gel capsules with a pitaya-like core-shell structure are constructed through a green polymerization strategy for pesticide detection and removal, namely ZIF-8/M-dbia/SA (M = Zn, Cd). Significantly, the ZIF-8/Zn-dbia/SA capsule exhibits sensitive detection of alachlor, a representative pre-emergence acetanilide pesticide, with a satisfactory detection limit of 0.23 µM. In addition, the MOF-based gel capsules can be extended to a universal visual platform for the noninvasive detection of pesticide residues with various MOFs, such as Eu-MOF, Tb-MOF, and Cu-MOF, and participating dye. Similar to pitaya, the ordered porous structure of MOF in ZIF-8/Zn-dbia/SA capsules offers cavity and open sites for removing pesticide from water with the maximum adsorption amount qmax of 61.1 mg·g-1 toward alachlor in a Langmuir model. Thereby, this work presents the universality of gel capsule self-assembly technologies, including the well-preserved visible fluorescence area and porosity of the different structurally diverse MOFs, offering an ideal strategy for water decontamination and food safety control fields.
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An interpenetrating structure endows metal-organic frameworks (MOFs) with many exciting applications, such as fluorescence detection and host-guest chemistry. Herein, two unique structure-interpenetrating In-MOFs (In-pdda-1 and In-pdda-2; H2pdda = 4,4'-(pyridine-2,5-diyl)dibenzoic acid) are constructed by different coordination configurations. The four-connected In3+ center shows a triangular-pyramidal configuration or a 2D rectangle, forming an unc topology for In-pdda-1 and a sql network for In-pdda-2, respectively. Two different interpenetrating modes created by linear rigid ligands and metal clusters are observed in the two MOFs (In-pdda-1, 8-fold interpenetrating mode; In-pdda-2, [2D + 2D] interpenetrating mode), which determine the channel-size-dependent properties in fluorescence applications. During the quantitative detection process of gossypol, the small rhombic channels divided by interpenetrating molecular planes of In-pdda-2 greatly limit the distance between the analyte and the probe, promoting electron transfer and energy transfer processes and thus resulting in a low detection limit (28.6 nM). In addition, the pore size effect of In-pdda-1 encouraged us to explore an in situ perovskite quantum dot encapsulation strategy to obtain a MAPbBr3@MOF material with tunable and stable luminescence properties. Both of the above channel-size-dependent fluorescence properties may provide inspiration for the structural design and specialized applications of MOF materials.
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Spiro-OMeTAD is the well-known hole transporting material (HTM) in perovskite solar cells. In this work, its derivatives, namely four D-A shaped triphenylamine or biphenylamine endcapped indenone spirofluorene (SFD-TPA, SFD-OMeTPA, SFD-TAD, and SFD-OMeTAD), were designed and synthesized. With the introduction of electron-donating moieties and the extension of conjugation length, a series of changes in photophysical and electrochemical properties could be detected. Notably, in comparison with the optical gap (2.96 eV) of the reported spiro-OMeTAD, SFD-OMeTAD presents an optical gap as low as 1.87 eV. Moreover, density functional theory simulations were employed to further investigate their geometric and electronic structures. Finally, steady-state photoluminescence measurements proved the efficient charge separation and collection processes at the perovskite/HTM interface. It can be predicted that all four compounds with enhanced sunlight absorption capability and suitable frontier energy levels can be used as hole-transporting materials for perovskite solar cells.
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Conventional oxidation of 2,2',7,7'-tetrakis[N,N-di(4-methoxyphenyl)amino]-9,9'-spirobifluorene (Spiro-OMeTAD) by air would bring various drawbacks for perovskite solar cells (PSCs), such as low power conversion efficiency (PCE) and poor stability. Here, a series of heteroatom-substituted Keggin-type polyoxometalates (POMs), H4PMo11VO40 (PMo11V), H5PMo10V2O40 (PMo10V2), and H6PMo9V3O40 (PMo9V3) are prepared and applied as p-type dopants to realize quantitative and controllable oxidation of Spiro-OMeTAD under an inert condition. The possible mechanism and electron donor regions in the oxidation of Spiro-OMeTAD are investigated using two-dimensional nuclear magnetic resonance (NMR) spectra and the relationship between POM structures and the oxidation degree of Spiro-OMeTAD is proposed. In addition, the synergistic effect of heteroatoms makes V2-substituted PMo10V2 exhibit appropriate oxidation of Spiro-OMeTAD and promoted the highest efficient hole extraction as well as the decreased charge recombination. Therefore, the champion device doped with PMo10V2 shows a PCE of 20.41% and a superior open circuit voltage (Voc) of 1.133 V, surpassing that of the pristine device (18.61%). This work presents a fresh perspective to the controllable oxidation of Spiro-OMeTAD employing economical inorganic POM dopants, which would promote the commercialization of PSCs.
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The immoderate use of pesticides in the modern agricultural industry has led to the pollution of water resources and ultimately threatens the human body. Herein, two metal-organic frameworks (MOFs), namely {[Zn(tpt)2 ·2H2 O]}n (Zn1) and {[Zn2 (tpt)2 (bdc)]}n (Zn2), (Htpt = 5-[4(1H-1,2,4-triazol-1-yl)]phenyl-2H-tetrazole), respectively, are constructed as smart materials for visual and on-site detection of pesticides and their removal from water. The exposed nitrogen-rich sites and high chemical stability make Zn2 a self-assembly core to further fabricate MOF-on-MOF-sodium alginate (ZIF-8-on-Zn2@SA) composite by wrapping ZIF-8 on the outside surface. Inheriting the excellent fluorescent emission of Zn2, the rod-like ZIF-8-on-Zn2@SA module exhibits naked-eye detection of thiophanate-methyl (TM) in real fruits and vegetables with a broad linear range (10-100 × 10-6 m), a low limit of detection (LOD = 0.14 × 10-6 m), and satisfactory recoveries (98.30-102.70%). In addition, carbendazim (CBZ), the metabolite of TM after usage in crops, can be efficiently removed from water by the ZIF-8-on-Zn2@SA (qmax = 161.8 mg g-1 ) with a high correlation coefficient (R2 > 0.99). Therefore, the portable ZIF-8-on-Zn2@SA sensing platform presents a promising candidate for monitoring and removal of pesticides, especially suitable for regions with serious pesticide environmental pollution.
Sujet(s)
Réseaux organométalliques , Pesticides , Alginates , Humains , Hydrogels , Pesticides/analyse , EauRÉSUMÉ
Pesticides have been emerged as major organic pollutants in environment, owing to widely spread and intrinsic high toxicity in agricultural productivity. Herein, we designed and synthesized a practicability and portable metal-organic framework (MOF) based composite beads MOF-alginate-Ca2+-polyacrylic acid (kgd-M1@ACPs) consist of biocompatible host material (sodium alginate) and fluorescent center with blue emission (where kgd-M1 stands for {[Cd(tbia)·H2O]·2H2O}n), which was further developed for high-efficiency and naked-eye 2,6-dichloro-4-nitroaniline (DCN) monitoring in fruits and vegetables. Significantly, the kgd-M1@ACPs shows obvious fluorescent quench towards toxic pesticide DCN with a low limit of detection (LOD) of 0.09 µM and high recovery from 98.08 to 104.37%. Moreover, the kgd-M1@ACPs also presents an excellent DCN adsorption ability. This work demonstrates that smart material kgd-M1@ACPs is expected to be a good candidate for detection and removal of DCN in real fruits and vegetables, which will present a broad prospect for monitoring and treating pesticides.
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Réseaux organométalliques , Pesticides , Alginates , Fruit , LégumesRÉSUMÉ
Ratiometric fluorescent probes based on coordination polymers (CPs) have been widely applied in optical applications. Therefore, it is very important to develop a dual-emitting gel material based on coordination polymers for specific recognition of molecules. Cu-atda (H2atda = 3,3'-(4-amino-1,2,4-triazol-3,5-diyl) dibenzoic acid) is synthesized with a porous structure and a large number of amino sites exposed on the surface, which can be regarded as a carrier for fluorescent molecules and well disperse in the SA hydrogel network. A dual-emission Eu3+ functionalized CP hydrogel bead (9A/Cu-atda@Eu3+/SA, 9A = 9-anthraldehyde and SA = sodium alginate) is successfully prepared, which presents ratiometric fluorescence detection of flumequine with a low detection limit (48 nM) and high selectivity. Furthermore, it also displays an excellent fluorescence quenching effect on nitrofuran antibiotics, exhibiting a dual functional performance. In addition, the fluorescence response mechanisms of flumequine and nitrofuran antibiotics are discussed in depth. As a portable material, visualization 9A/Cu-atda@Eu3+/SA beads provide an extensive and convenient application prospect for real-time monitoring of antibiotics in the water environment.
Sujet(s)
Colorants fluorescentsRÉSUMÉ
Stimuli-responsiveness is an important characteristic that show promising potential in various applications. Herein, a novel ZIF-8-on-Tb-dpn (H3dpn = 5-(2',4'-dicarboxylphenyl)nicotic acid) heterostructure is constructed using a heteroepitaxial strategy combining the chemical-responsive (antibiotics) and light-responsive behaviors. The pyridine nitrogen of Tb-dpn acts as an anchor site for Zn2+, which helps to overcome the limit of lattice mismatch between two metal-organic frameworks (MOFs) and promotes the growth of ZIF-8 nanocrystals. Based on the synergy effect of two MOFs, ZIF-8-on-Tb-dpn exhibits an efficient turn-off response toward tetracycline and chloramphenicol via competitive absorption, Förster resonance energy transfer, and photoinduced electron transfer processes with limit of detection values of 5.6 and 37.6 nM, respectively, which are three- to -fivefold lower than those of Tb-dpn. Moreover, the nanocage of ZIF-8 is utilized to encapsulate photochromic spiropyran (SP) molecules and realize the reversible conversion between SP and merocyanine (MC) under visible light and ultraviolet light. The MC form is accompanied with strong adsorption at 555 nm, which can erase the emission of Tb3+. Therefore, a reversible invisible anticounterfeiting pattern is designed with SP â ZIF-8-on-Tb-dpn for information anticounterfeiting. The excellent stimuli-responsive ability makes the luminescent platform a potential candidate in luminescence applications.
Sujet(s)
Antibactériens/analyse , Escroquerie/prévention et contrôle , Luminescents/composition chimique , Réseaux organométalliques/composition chimique , Adsorption , Antibactériens/composition chimique , Chloramphénicol/analyse , Chloramphénicol/composition chimique , Indoles/composition chimique , Indoles/effets des radiations , Isomérie , Spiranes/composition chimique , Spiranes/effets des radiations , Tétracycline/analyse , Tétracycline/composition chimique , Rayons ultravioletsRÉSUMÉ
Metal-organic frameworks (MOFs)-based sensors for monitoring toxic substances in wastewater have attracted great attention due to the efficient and reliable performance. Here, we has synthesized two novel zinc-based MOFs [Zn(ttb)2(H2O)2]n (Zn1-ttb) and {[Zn(ttb)2]·0.5CH3CN}n (Zn2-ttb) through changing the polarity of reaction solvents and finally obtained target 2D MOF material [Zn(ttb)(bdc)0.5]n(Zn3-ttb-bdc) by successfully introducing an ancillary ligand H2bdc (Httb = 1-(triazo-1-ly)-4-(tetrazol-5-ylmethyl)benzene, H2bdc = 1,4-benzenedicarboxylic acid). As-prepared Zn3-ttb-bdc exhibits high water and chemical stability as well as excellent fluorescence property. Due to the -COOH binding sites from H2bdc, Zn3-ttb-bdc shows high sensitivity and a rapid luminescent response to a representative organic micropollutant trinitrophenol (TNP) and inorganic pollutants (Fe3+ and Cr2O72-) in wastewater. The mechanisms of multifunctional detection abilities of Zn3-ttb-bdc toward different types of pollutants are further studied. This work presents the structural design in preparing MOF materials for multifunctional detection performance, thus opening new perspectives for emerging MOF-based sensors as environmental monitors.
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A special functional group mediated functionalization platform is introduced as a new and versatile platform tool to improve the fluorescence detection performance of metal-organic frameworks (MOF). The creation of a mixed-functionalization strategy on a MOF realizes the high sensitivity detection of heavy metal ions, anions and small molecules. In this work, we have first reported a novel amino functionalized 3D indium MOF [In(BDC-NH2)(OH)]n (In1-NH2) which not only has an excellent fluorescent characteristic but also shows highly sensitive identification of Fe3+, Cu2+, Pb2+ and ClO- in water with broad linear ranges and short response times. Subsequently, based on the remaining amino group site of In1-NH2, a post-synthetic modification strategy is utilized to introduce an active boronic acid group for hydrogen peroxide detection. The obtained PBA-In1 exhibits an efficient sensing performance for hydrogen peroxide with an LOD of 0.42 µM. Given this, PBA-In1 is expected to become an effective probe to monitor the formation of metabolites in humans. In1-NH2 successfully achieves multiple ion detection and the PBA-In1 sensing platform with boronic acid functionalization may have good application prospects in biochemical research in the future.
Sujet(s)
Acides boroniques/composition chimique , Peroxyde d'hydrogène/analyse , Acide hypochloreux/analyse , Réseaux organométalliques/composition chimique , Métaux lourds , Acides phtaliques/composition chimique , Polluants chimiques de l'eau/analyse , Marqueurs biologiques/analyse , Surveillance de l'environnement , Fluorescence , Métaux lourds/analyse , Métaux lourds/composition chimiqueRÉSUMÉ
Currently, Spiro-OMeTAD is the most widely used hole transport material (HTM) in the best-performing perovskite solar cells (PSCs), resulting from its suitable energy level and facile processing. However, the intrinsic properties of organic molecules, such as low conductivity and a nonpolar contact interface, will limit the power conversion efficiency (PCE) and stability of Spiro-OMeTAD-based PSCs. Chemical doping could be an effective strategy to ameliorate the performance of Spiro-OMeTAD, and most of the dopants are designed for controllably oxidizing Spiro-OMeTAD. In this work, a highly stable metal-organic framework {[Zn(Hcbob)]·(solvent)}n (Zn-CBOB) with rod topology and Lewis basic sites is assembled and employed as a dopant for the hole transport layer. It is found that Zn-CBOB not only controllably oxidizes Spiro-OMeTAD and improves the conductivity of the HTM but also passivates the surface traps of the perovskite film by coordinating with Pb2+. The Zn-CBOB-doped PSCs achieved a remarkable PCE of 20.64%. In addition, the hydrophobicity of Zn-CBOB can prevent water from destroying the perovskite layer, which helps elevate the stability of PSCs.
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Chemical doping engineering is an effective strategy to modify the hole transport layer (HTL) and achieve high-efficiency perovskite solar cells (PSCs). In this work, we synthesize an infrequent trilacunary Keggin type polyoxometalate Na10[Zn2(H2O)6(WO2)2(BiW9O33)2] (BiW9-Zn) and apply it as an additive to enhance the hole mobility and electrical conductivity of Spiro-OMeTAD based HTLs. Thanks to the strong electron-accepting properties of polyoxometalate molecules, the as-synthesized BiW9-Zn can directly oxidize Spiro-OMeTAD under an inert atmosphere and avoid the tedious long-term oxidation process. Therefore, the power conversion efficiency (PCE) of optimal PSCs with BiW9-Zn doping is enhanced from 17.58% (without doping) to 19.56% with a significantly improved fill factor and open-circuit voltage. In addition, the assembly repeatability and long-term stability of PSCs are also improved. This work demonstrates the potential of using polyoxometalates (POMs) as low-cost, efficient and highly flexible chemical dopants for HTLs, and more importantly paves a new route to enhance the performance of PSCs.
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Developing portable membrane sensors to accurately detect the biomolecule ascorbic acid (AA) is extremely important for food safety and human health. Herein, we successfully design and synthesize a novel cationic metal organic framework (Eu-pbmc, Hpbmc = 2-(pyridine-2-yl)-1H-benzimidazole-5-carboxylic acid) and assemble polyacrylonitrile/Eu-pbmc membrane (PEM) by an in-situ growth strategy. Benefiting from the appreciable loading of Eu-pbmc nanoparticles and high water permeation flux, PEM possesses effective detection for MnO4- with a limit of detection (LOD) of 17 nM. Utilizing the cationic porous framework, we load MnO4- into PEM and construct a "on-off-on" system for effective AA detection. The oxidative MnO4- can be reduced by AA and the resulting turn-on luminescence can reflect the concentration of AA. Compared with pure Eu-pbmc crystals, PEM exhibits improved AA detection performance with LOD of 48 nM and detection time of 1 min via a concise detection operation. The stable membrane sensor realizes an accurate detection in real biological samples, meeting the practical requirement. Moreover, an IMP logic gate is helpful to analyze MnO4- and AA in water. The proposed novel luminescence platform as well as reasonable "on-off-on" luminescence mode provide a promising method for AA detection.
Sujet(s)
Lanthanides , Réseaux organométalliques , Acide ascorbique , Humains , Agranulocytes , LuminescenceRÉSUMÉ
Accurate hydrophobicity adjustment of single-phase material is quite challenging and meaningful for water treatment. Here, a strategy combining crystal morphology regulation and post-synthetic modification is reported based on a novel metal-organic framework (MOF, Eu-bdo-COOH, H4bdo = 2,5-bis(3,5-dicarboxylphenyl)-1,3,4-oxadiazole). The hydrophobicity is regulated by crystal size and morphology regulation, and a rough microspherical MOF is successfully synthesized. Meanwhile, the obtained MOF microspheres exhibit high water, chemical, and thermal stability. The post-synthetic modification of alkyl chains achieves fine-tuning of hydrophobicity of MOF microspheres. The static water contact angles can controllably range from 43 to 142°, and the amylamine-modified MOF (AM) obtains the strongest hydrophobicity. In addition, a superhydrophobic aerogel is constructed with AM microspheres and reduced graphene oxide (rGO) for efficient oil-water separation. The AM-rGO aerogel (AM-rGA) exhibits fast and efficient absorption of various oily substances from water, and the adsorption capacity of dibromoethane reaches up to 14,728 wt %. This outstanding oil adsorption capacity can maintain even beyond 50 cycles by the support of the stable aerogel. The strategy of morphology regulation and post-synthetic modification provides a broad approach for the hydrophobic adjustment of numerous MOF materials.
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It is very significant that functional porous metal-organic frameworks are used to manufacture hierarchical components to achieve cascading functions that cannot be achieved by a single-layer metal-organic framework (MOF). Here, we report two cases of novel MOFs constructed by the same ligand, Cu(I)-tpt and Cu(II)-tpt (Htpt = 5-[4(1H-1,2,4-triazol-1-yl)]phenyl-2H-tetrazole), and prepared a Cu(II)-tpt-on-Cu(I)-tpt membrane by a layer-by-layer approach ignoring the lattice mismatch problem. The first Cu(I)-tpt layer is grown on an oriented Cu2O nanostructured array by a "one-pot" approach. The aligned second Cu(II)-tpt layer can be deposited using liquid-phase epitaxy. Notably, the prepared Cu(II)-tpt-on-Cu(I)-tpt membrane combines adsorption and fluorescence sensing, which exhibited significant adsorption for Cr2O72- (203.25 mg g-1) as typical highly poisonous ions with a fluorescence quenching response. Hence, based on the oxidation-reduction between Cr2O72- and p-arsanilic acid (p-ASA), the Cu(II)-tpt-on-Cu(I)-tpt membrane's ability to adsorb Cr2O72- could be used to design "on-off-on" mode fluorescence probes to detect p-ASA with high sensitivity (limit of detection (LOD) = 0.0556 µg L-1). p-ASA can be degraded into highly toxic inorganic arsenic compounds in the natural environment and has received widespread attention. Therefore, the integration of adsorption and fluorescence properties makes the Cu(II)-tpt-on-Cu(I)-tpt membrane a feasible multifunctional material for pollution control and detection.
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Three-dimensional (3D) porous carbon materials have received substantial attention owing to their unique structural features. However, the synthesis of 3D porous carbon, especially 3D porous carbon with hollow spheres structures at the connection points, still pose challenges. Herein, we first develop a metal-organic complexes@melamine foam (MOC@MF) template strategy, by using hot-pressing and carbonization method to synthesize 3D porous carbon with hollow spheres structures (denoted as NOPCs). The formation mechanism of NOPCs can be attributed to the difference in Laplace pressure and surface energy gradient between the carbonized MOC and carbonized MF. These rare 3D porous carbons exhibit high BET surface area (2453.8 m2 g-1), N contents (10.5%), and O contents (16.3%). Moreover, NOPCs show significant amounts of toluene and methanol at room temperature, reaching as high as 1360 and 1140 mg g-1. The adsorption amounts of SO2 and CO2 for NOPCs are up to 93.1 and 445 mg g-1. Theoretical calculation indicates surfaces of porous carbon with N and O coexistence could strongly enhance adsorption with high adsorption energy of -65.83 kJ mol g-1.