Thermal and photothermal catalytic selective oxidation of isobutane to methacrylic acid (MAA) are comparatively studied over a keggin-type Cs2.9Cu0.34V0.49PMo12O40 heteropolyacid acid. An introduction of light was observed to enhance both the i-C4H10 conversion and the MAA selectivity, and consequently the MAA formate rate, particularly at low temperatures. Characterization results show that oxidation of methacrolein (MAL) to MAA is the rate-limiting step while UV light illumination promotes the oxidation of σ-bonded MAL with OH groups to σ-bonded MAA on the catalyst surface. These results demonstrate a synergistic effect of thermal catalysis and photocatalysis in selective oxidation of isobutane to MAA, which suggests photothermal catalysis as a promising strategy to catalyze the selective oxidation of higher hydrocarbons at relative mild reaction conditions.
{"title":"Photothermal catalytic selective oxidation of isobutane to methacrylic acid over keggin-type heteropolyacid","authors":"Yichuan Wang, Xiao Sun, Zeyue Wei, Xuanyu Zhang, Weixin Huang","doi":"10.1063/1674-0068/cjcp2305056","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2305056","url":null,"abstract":"Thermal and photothermal catalytic selective oxidation of isobutane to methacrylic acid (MAA) are comparatively studied over a keggin-type Cs2.9Cu0.34V0.49PMo12O40 heteropolyacid acid. An introduction of light was observed to enhance both the i-C4H10 conversion and the MAA selectivity, and consequently the MAA formate rate, particularly at low temperatures. Characterization results show that oxidation of methacrolein (MAL) to MAA is the rate-limiting step while UV light illumination promotes the oxidation of σ-bonded MAL with OH groups to σ-bonded MAA on the catalyst surface. These results demonstrate a synergistic effect of thermal catalysis and photocatalysis in selective oxidation of isobutane to MAA, which suggests photothermal catalysis as a promising strategy to catalyze the selective oxidation of higher hydrocarbons at relative mild reaction conditions.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"56 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136199704","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-08-01DOI: 10.1063/1674-0068/cjcp2207111
Shiyan Cao, Sulei Hu, Wei-Xue Li
Revealing the fundamental mechanisms governing reactant-induced disintegration of supported metal nanoparticles and their dependences on the metal component and reactant species is vital for improving the stability of supported metal nanocatalysts and single-atom catalysts. Here we use first-principles based disintegration thermodynamics to study the CO- and OH- induced disintegration of Ag, Cu, Au, Ni, Pt, Rh, Ru, and Ir nanoparticles into metal-reactant complexes (M(CO)n, M(OH)n, n=1 and 2) on the pristine and bridge oxygen vacancy site of TiO2(110). It was found that CO has a stronger interaction with these considered transition metals compared to OH, resulting in lower formation energy and a larger promotion effect on the disintegration of nanoparticles (NPs). The corresponding reactant adsorption energy shows a linear dependence on the metal cohesive energy, and metals with higher cohesive energies tend to have higher atomic stability due to their stronger binding with reactant and support. Further disintegration free energy calculations of NPs into metal-reactant complexes indicate only CO-induced disintegration of Ni, Rh, Ru, and Ir nanoparticles is thermodynamically feasible. These results provide a deeper understanding of reactant-induced disintegration of metal nanoparticles into thermodynamically stable metal single-atom catalysts.
{"title":"First-principles thermodynamics study of CO/OH induced disintegration of precious metal nanoparticles on TiO2(110)","authors":"Shiyan Cao, Sulei Hu, Wei-Xue Li","doi":"10.1063/1674-0068/cjcp2207111","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2207111","url":null,"abstract":"Revealing the fundamental mechanisms governing reactant-induced disintegration of supported metal nanoparticles and their dependences on the metal component and reactant species is vital for improving the stability of supported metal nanocatalysts and single-atom catalysts. Here we use first-principles based disintegration thermodynamics to study the CO- and OH- induced disintegration of Ag, Cu, Au, Ni, Pt, Rh, Ru, and Ir nanoparticles into metal-reactant complexes (M(CO)n, M(OH)n, n=1 and 2) on the pristine and bridge oxygen vacancy site of TiO2(110). It was found that CO has a stronger interaction with these considered transition metals compared to OH, resulting in lower formation energy and a larger promotion effect on the disintegration of nanoparticles (NPs). The corresponding reactant adsorption energy shows a linear dependence on the metal cohesive energy, and metals with higher cohesive energies tend to have higher atomic stability due to their stronger binding with reactant and support. Further disintegration free energy calculations of NPs into metal-reactant complexes indicate only CO-induced disintegration of Ni, Rh, Ru, and Ir nanoparticles is thermodynamically feasible. These results provide a deeper understanding of reactant-induced disintegration of metal nanoparticles into thermodynamically stable metal single-atom catalysts.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"30 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135004002","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-08-01DOI: 10.1063/1674-0068/36/04/cabs
{"title":"Chinese Abstracts","authors":"","doi":"10.1063/1674-0068/36/04/cabs","DOIUrl":"https://doi.org/10.1063/1674-0068/36/04/cabs","url":null,"abstract":"","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"24 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135003999","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-08-01DOI: 10.1063/1674-0068/cjcp2110215
Hai-Zhen Yu, Li Wang, Chuan-Kui Wang, Zhen Xie
The oxygen reduction reaction (ORR) by the nitrogen-doped fullerene (C59N) catalyst demonstrates an excellent activity in hydrogen fuel cells. However, the intermediates and catalytic active sites in pathways have not been directly characterized, hindering the understanding of the enhanced activity mechanism for ORR on C59N. By taking the inhomogeneity of spatially confined plasmon into account, we theoretically propose that the high-resolution tip-enhanced Raman scattering (TERS) can effectively identify different intermediate configurations in ORR on C59N. With the modulation of the focused spatially confined plasmon center position, vibrational modes that are directly related to site-specific O2-C59N interactions in ORR can be lighted up and then selected out by TERS spectra. Furthermore, the vibration-resolved TERS images for the selected modes of different intermediate configurations give spatial hot spot around the adsorption site, providing the in-situ details of catalytic active sites in ORR on C59N. These findings serve as a good reference for future high-resolution TERS experiments on probing catalytic systems at the molecular scale.
{"title":"Identifying intermediates of oxygen reduction reaction on nitrogen-doped fullerene by high-resolution tip-enhanced Raman scattering","authors":"Hai-Zhen Yu, Li Wang, Chuan-Kui Wang, Zhen Xie","doi":"10.1063/1674-0068/cjcp2110215","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2110215","url":null,"abstract":"The oxygen reduction reaction (ORR) by the nitrogen-doped fullerene (C59N) catalyst demonstrates an excellent activity in hydrogen fuel cells. However, the intermediates and catalytic active sites in pathways have not been directly characterized, hindering the understanding of the enhanced activity mechanism for ORR on C59N. By taking the inhomogeneity of spatially confined plasmon into account, we theoretically propose that the high-resolution tip-enhanced Raman scattering (TERS) can effectively identify different intermediate configurations in ORR on C59N. With the modulation of the focused spatially confined plasmon center position, vibrational modes that are directly related to site-specific O2-C59N interactions in ORR can be lighted up and then selected out by TERS spectra. Furthermore, the vibration-resolved TERS images for the selected modes of different intermediate configurations give spatial hot spot around the adsorption site, providing the in-situ details of catalytic active sites in ORR on C59N. These findings serve as a good reference for future high-resolution TERS experiments on probing catalytic systems at the molecular scale.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"46 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135004000","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/36/03/cabs
{"title":"Chinese Abstracts","authors":"","doi":"10.1063/1674-0068/36/03/cabs","DOIUrl":"https://doi.org/10.1063/1674-0068/36/03/cabs","url":null,"abstract":"","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"28 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"136350426","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/cjcp2205093
Xiaojun Wang, Ni Lu, Yuan C. Fu, Ch. Lu, Meili Guan, Kunhua Wang, Hao Yu
The 5-hydroxymethylfurfural (5-HMF) acts as an important chemical intermediate to bridge the biomass resources and industrial applications, which shows the potential for green development. However, the performance of biomass materials conversion to 5-HMF is still limited in the green solvent. Herein, an effective approach is reported to prepare the highly efficient solid acid catalysts, NbOx/WOy-ZrO2, to improve fructose conversion. It is found that the introduction of Nb results in the generation of the niobium oxides, which improves acid sites and tunes the ratios of Brønsted acid and Lewis acid on the surface of the WOy-ZrO2 support. With the acidity improvement and increasing acid sites of the NbOx/WOy-ZrO2, the highest fructose conversion is 99% in water. Meanwhile, the 5-HMF yield and the selectivity are also as high as 50.1% and 50.7% under the reaction temperature of 180 °C for a short reaction time of 30 min. The proposed NbOx/WOy-ZrO2 catalyst strategy will not only open a new way for designing the solid acid catalysts to achieve high performance of the 5-HMF in the water, but also promote the green production of biomass and sustainable development in the future.
{"title":"Improved surface acidity of niobium doped tungstated-zirconia solid acid catalyst over production of 5-hydroxymethylfurfural","authors":"Xiaojun Wang, Ni Lu, Yuan C. Fu, Ch. Lu, Meili Guan, Kunhua Wang, Hao Yu","doi":"10.1063/1674-0068/cjcp2205093","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2205093","url":null,"abstract":"The 5-hydroxymethylfurfural (5-HMF) acts as an important chemical intermediate to bridge the biomass resources and industrial applications, which shows the potential for green development. However, the performance of biomass materials conversion to 5-HMF is still limited in the green solvent. Herein, an effective approach is reported to prepare the highly efficient solid acid catalysts, NbOx/WOy-ZrO2, to improve fructose conversion. It is found that the introduction of Nb results in the generation of the niobium oxides, which improves acid sites and tunes the ratios of Brønsted acid and Lewis acid on the surface of the WOy-ZrO2 support. With the acidity improvement and increasing acid sites of the NbOx/WOy-ZrO2, the highest fructose conversion is 99% in water. Meanwhile, the 5-HMF yield and the selectivity are also as high as 50.1% and 50.7% under the reaction temperature of 180 °C for a short reaction time of 30 min. The proposed NbOx/WOy-ZrO2 catalyst strategy will not only open a new way for designing the solid acid catalysts to achieve high performance of the 5-HMF in the water, but also promote the green production of biomass and sustainable development in the future.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":" ","pages":""},"PeriodicalIF":1.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"46154589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/cjcp2304042
Xinlei Chen, Guanjun Wang, Weixing Li
The characterization of the structures of molecular clusters, which serve as building blocks for bulk substances, provides crucial insight into the interactions between constituent units. Chirped-pulse Fourier transform microwave (CP-FTMW) spectroscopy, combined with state-of-the-art quantum chemical calculations, is a powerful tool for characterizing the structures of molecular clusters, as the rotational spectra are directly related to the mass distribution of a molecule or cluster. However, determining the structures of large or complex clusters from experimental rotational spectra remains challenging due to their structural flexibility. Ab initio and density functional theory calculations for searching their stable structures could be significantly time-consuming and method-dependent. To address these challenges, we have developed an approach that relies on the experimental rotational constants to search for potential molecular structures without quantum chemical optimization. Our approach involves creating an initial set of conformers through either a semi-empirical sampling program or the quasi-Monte Carlo method. After-ward, the trust region reflective algorithm is utilized for structure fitting. This procedure enables us to quickly generate potential conformers and gain access to precise structural information. We apply our fitting program to water hexamer and benzaldehyde-water clusters, and the resulting topological structures align extremely well with the experimental results.
{"title":"A fitting program for structural determination of molecular clusters from rotational spectroscopy","authors":"Xinlei Chen, Guanjun Wang, Weixing Li","doi":"10.1063/1674-0068/cjcp2304042","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2304042","url":null,"abstract":"The characterization of the structures of molecular clusters, which serve as building blocks for bulk substances, provides crucial insight into the interactions between constituent units. Chirped-pulse Fourier transform microwave (CP-FTMW) spectroscopy, combined with state-of-the-art quantum chemical calculations, is a powerful tool for characterizing the structures of molecular clusters, as the rotational spectra are directly related to the mass distribution of a molecule or cluster. However, determining the structures of large or complex clusters from experimental rotational spectra remains challenging due to their structural flexibility. Ab initio and density functional theory calculations for searching their stable structures could be significantly time-consuming and method-dependent. To address these challenges, we have developed an approach that relies on the experimental rotational constants to search for potential molecular structures without quantum chemical optimization. Our approach involves creating an initial set of conformers through either a semi-empirical sampling program or the quasi-Monte Carlo method. After-ward, the trust region reflective algorithm is utilized for structure fitting. This procedure enables us to quickly generate potential conformers and gain access to precise structural information. We apply our fitting program to water hexamer and benzaldehyde-water clusters, and the resulting topological structures align extremely well with the experimental results.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":" ","pages":""},"PeriodicalIF":1.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49271842","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/cjcp2304041
Z. Luan, Yanlin Fu, Yuxin Tan, Yaling Wang, An-wen Liu, Tao Wang, Xiaoguo Zhou, Bina Fu, Dong H. Zhang, Daofu Yuan, Xingan Wang, Xueming Yang
We study the photodissociation dynamics of the hydrogen sulfide cations (H2S+) using the time-sliced velocity map ion imaging (VMI) technique and high-accuracy calculations. High-resolution ion images of the S+(4S) products were measured at four photolysis wavelengths of 325.158, 325.200, 325.243, 325.307 nm, which correspond to the excitation to the A2A1(0,13,0) K=1 state of H2S+. Rotational state-resolved total kinetic energy releases and angular distributions have been derived as a function of the photolysis wavelengths. Notably, photolysis wavelength dependent product rotational state and anisotropy parameter distributions have been clearly observed. Full-dimensional potential energy surface characterization suggests that nonadiabatic coupling between A2A1 and B2B2 states at C2v configurations, as well as relaxation of the symmetry to Cs in the conical intersection region between the two states, plays a key role in the photodissociation process.
{"title":"Photodissociation dynamics of H2S+ near 325 nm","authors":"Z. Luan, Yanlin Fu, Yuxin Tan, Yaling Wang, An-wen Liu, Tao Wang, Xiaoguo Zhou, Bina Fu, Dong H. Zhang, Daofu Yuan, Xingan Wang, Xueming Yang","doi":"10.1063/1674-0068/cjcp2304041","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2304041","url":null,"abstract":"We study the photodissociation dynamics of the hydrogen sulfide cations (H2S+) using the time-sliced velocity map ion imaging (VMI) technique and high-accuracy calculations. High-resolution ion images of the S+(4S) products were measured at four photolysis wavelengths of 325.158, 325.200, 325.243, 325.307 nm, which correspond to the excitation to the A2A1(0,13,0) K=1 state of H2S+. Rotational state-resolved total kinetic energy releases and angular distributions have been derived as a function of the photolysis wavelengths. Notably, photolysis wavelength dependent product rotational state and anisotropy parameter distributions have been clearly observed. Full-dimensional potential energy surface characterization suggests that nonadiabatic coupling between A2A1 and B2B2 states at C2v configurations, as well as relaxation of the symmetry to Cs in the conical intersection region between the two states, plays a key role in the photodissociation process.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":" ","pages":""},"PeriodicalIF":1.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"49005833","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/cjcp2104071
Antony Minja, Taotao Wang, Hongyun Cao, Pingwu Du
Herein, we present the decoration of NiFeCoAlOOH nanoparticles onto titanium doped nanoporous hematite (Ti-PH) utilizing a simple electroless ligand-controlled oxidation method for photoelectrochemical water splitting. Owing to the improved oxygen evolution reaction kinetics and reduced charge transfer resistance, the resulting Ti-PH/NiFeCoAlOOH photoanode presents an excellent photocurrent density of 2.46 mA/cm2 at 1.23 V vs. RHE and good stability compared to Ti-PH or bare hematite. Furthermore, the onset potential of the photocurrent density is shifted cathodically by ∼60 mV with reference to the titanium doped nanoporous hematite. This work offers a promising method for designing high-performance, stable, and inexpensive catalysts for photoelectrochemical applications.
{"title":"Titanium doped nanoporous hematite photoanode modified with NiFeCoAlOOH nanoparticles for efficient photoelectrochemical water splitting","authors":"Antony Minja, Taotao Wang, Hongyun Cao, Pingwu Du","doi":"10.1063/1674-0068/cjcp2104071","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2104071","url":null,"abstract":"Herein, we present the decoration of NiFeCoAlOOH nanoparticles onto titanium doped nanoporous hematite (Ti-PH) utilizing a simple electroless ligand-controlled oxidation method for photoelectrochemical water splitting. Owing to the improved oxygen evolution reaction kinetics and reduced charge transfer resistance, the resulting Ti-PH/NiFeCoAlOOH photoanode presents an excellent photocurrent density of 2.46 mA/cm2 at 1.23 V vs. RHE and good stability compared to Ti-PH or bare hematite. Furthermore, the onset potential of the photocurrent density is shifted cathodically by ∼60 mV with reference to the titanium doped nanoporous hematite. This work offers a promising method for designing high-performance, stable, and inexpensive catalysts for photoelectrochemical applications.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"45 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135219501","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2023-06-01DOI: 10.1063/1674-0068/cjcp2106103
Kangkang He, Fei Hu, Chaoshi Chen, M. Atif, Yanmei Wang
Mixed polymer brushes coating based on poly (2-methyl-2-oxazoline)/ poly(4-vinyl pyridine) (PMOXA/P4VP) was prepared by simultaneously grafting amine-terminated PMOXA and thiolterminated P4VP onto poly(dopamine) (PDA)-modified substrates in this work. The coatings were characterized by X-ray photoelectron spectroscopy, ellipsometry, zeta potential measurements, and the static water contact angle tests. The results indicated that it is feasible to control the components of the coating by adjusting the feed ratio of PMOXA to P4VP. Moreover, the zeta potential and the water contact angle of mixed brushes modified surfaces could be tuned by changing the environmental pH value and surface compositions. Finally, fluorescein isothiocyanate-labelled pepsin assay and surface plasmon resonance were performed to investigate the responsive adsorption/desorption of pepsin by PMOXA/P4VP mixed brushes. The results showed that by adjusting the fraction of PMOXA or P4VP, the PMOXA/P4VP mixed brushes coated surfaces could adsorb a high amount of pepsin at pH=3, and achieve a desorption efficiency of over 92% at pH=7.
{"title":"Polydopamine anchored poly(2-methyl-2-oxazoline)/poly(4-vinyl pyridine) mixed brushes with switchable properties for pepsin adsorption","authors":"Kangkang He, Fei Hu, Chaoshi Chen, M. Atif, Yanmei Wang","doi":"10.1063/1674-0068/cjcp2106103","DOIUrl":"https://doi.org/10.1063/1674-0068/cjcp2106103","url":null,"abstract":"Mixed polymer brushes coating based on poly (2-methyl-2-oxazoline)/ poly(4-vinyl pyridine) (PMOXA/P4VP) was prepared by simultaneously grafting amine-terminated PMOXA and thiolterminated P4VP onto poly(dopamine) (PDA)-modified substrates in this work. The coatings were characterized by X-ray photoelectron spectroscopy, ellipsometry, zeta potential measurements, and the static water contact angle tests. The results indicated that it is feasible to control the components of the coating by adjusting the feed ratio of PMOXA to P4VP. Moreover, the zeta potential and the water contact angle of mixed brushes modified surfaces could be tuned by changing the environmental pH value and surface compositions. Finally, fluorescein isothiocyanate-labelled pepsin assay and surface plasmon resonance were performed to investigate the responsive adsorption/desorption of pepsin by PMOXA/P4VP mixed brushes. The results showed that by adjusting the fraction of PMOXA or P4VP, the PMOXA/P4VP mixed brushes coated surfaces could adsorb a high amount of pepsin at pH=3, and achieve a desorption efficiency of over 92% at pH=7.","PeriodicalId":10036,"journal":{"name":"Chinese Journal of Chemical Physics","volume":"1 1","pages":""},"PeriodicalIF":1.0,"publicationDate":"2023-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"58525812","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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