Article(id=1320090130614961042, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320090116236882876, articleNumber=null, orderNo=null, doi=10.14062/j.issn.0454-5648.20240571, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=null, receivedDate=1724947200000, receivedDateStr=2024-08-30, revisedDate=1726761600000, revisedDateStr=2024-09-20, acceptedDate=null, acceptedDateStr=null, onlineDate=1792663613226, onlineDateStr=2026-10-22, pubDate=1745078400000, pubDateStr=2025-04-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1792663613226, onlineIssueDateStr=2026-10-22, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1792663613226, creator=13701087609, updateTime=1792663613226, updator=13701087609, issue=Issue{id=1320090116236882876, tenantId=1146029695717560320, journalId=1263187385517883426, year='2025', volume='53', issue='4', pageStart='733', pageEnd='1030', issueExtLink='null', onlineDate='null', pubDate='1745078400000', pubDateStr='2025-04-20', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1792663609799, creator='13701087609', updateTime=1792663788359, updator='13701087609', preIssue=null, nextIssue=null, articleTotal=null, ext={EN=IssueExt(id=1320090865276670951, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320090116236882876, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1320090865276670952, tenantId=1146029695717560320, journalId=1263187385517883426, issueId=1320090116236882876, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null, downloadFileDto=null}, startPage=839, endPage=848, ext={EN=ArticleExt(id=1320090130816287635, articleId=1320090130614961042, tenantId=1146029695717560320, journalId=1263187385517883426, language=EN, title=Stability and Mechanism of SiO
2 Modified Ag
10Si
4O
13/GO for Photocatalytic Degradation of Methylene Blue, columnId=1321897768591937660, journalTitle=Journal of the Chinese Ceramic Society, columnName=Special Issue on the 14th Inorganic and Non-metallic Materials Conference—Research Article, runingTitle=null, highlight=null, articleAbstract=
Introduction A photocatalytic material of Ag10Si4O13 is widely concerned due to its band structure suitable for visible light response and built-in electric field promoting photogenerated carrier separation. However, in the photocatalysis process, Ag+ in Ag10Si4O13 is easily reduced by photoelectrons and accumulates Ag elements, affecting the cycle stability of the photocatalytic system. Graphene oxide can effectively transfer photogenerated electrons, and amorphous SiO2 can inhibit ion diffusion leaching, which are expected to slow down the photoreduction of Ag10Si4O13. In this paper, x% SiO2/Ag10Si4O13/GO (SAG) composites with different amounts of amorphous SiO2 were prepared via adding graphene oxide (GO) and silica sol in the process of Ag10Si4O13 preparation by a sol-gel method. The effect of amorphous SiO2 addition on the crystal structure, morphology and photoelectrochemical properties was investigated. Methylene blue (MB) was used as a target. The results show that a small amount of amorphous SiO2 can greatly improve the photoreduction resistance of Ag10Si4O13 photocatalysts, and broaden the photoresponse range and increase the adsorption capacity of the material for MB. However, the addition of amorphous SiO2 can simultaneously reduce the migration rate of photogenerated carriers and accelerate the recombination of photogenerated electron-hole pairs. Therefore, the photocatalytic degradation efficiency of the composite system firstly increases and then decreases with the increase of SiO2 addition. The degradation rate of SiO2/Ag10Si4O13/GO (SAG-1) samples can reach 99% under visible light for 40 min, showing a good cyclic stability. After 5 cycles, the crystal structure of the materials becomes stable and the degradation rate can still reach 97%.
Methods In pre-hydrolysis of ethyl orthosilicate: 0.47 g of citric acid was added to 26 mL of anhydrous ethanol under magnetic stirring until complete dissolution, and then 5 mL of ethyl orthosilicate and 1.65 mL of distilled water were added in dropwise to the solution and the solution was stirred for 1 h and sealed for 1 week aging to obtain the silica sol. In preparation of Ag10Si4O13/GO, 2.1 mL of silica sol and GO sol containing 1%(in mass) Ag10Si4O13 were added to 10 mL of distilled water under ultrasound and magnetic stirring. 1.6 mL of 0.38 g/mL AgNO3 solution was added in dropwise to the mixed solution above under stirring for 1 h and aging for 24 h to obtain the precursor sol. The precursor sol was dried, ground and heat-treated at 400 ℃ for 5 h to obtain a brick-red Ag10Si4O13/GO powder=(i.e., AG). In preparation of SiO2/Ag10Si4O13/GO, x%(in mass) Ag10Si4O13 (x=1, 2, 3, 4) of silica sol was added, stirred continuously for 1 h and aged for 24 h to obtain x% SiO2/Ag10Si4O13/GO precursor sol. The subsequent steps were the same as for AG to obtain x% SiO2/Ag10Si4O13/GO powders (i.e., SAG-1, SAG-2, SAG-3, and SAG-4), respectively.
The crystal structure of the materials was characterized by a model D8/axs X-ray diffractometer (XRD, Bruker Co., Germany). The microscopic morphology of the materials was observed by a model JSM-6701F transmission electron microscope (TEM, Electro-Optics Co., Japan). The chemical state was analyzed by a model PHI5702 X-ray photoelectron spectrometer (XPS, Physical Electronics Inc., USA). The photoresponsive properties were determined by a model U-3900H diffuse reflectance spectrometer (UV-Vis, Hitachi High-Technologies Co., Japan). The fluorescence emission spectra of the materials were determined by a model F97 fluorescence spectrophotometer (FSP, Shanghai Prismatic Technology Co., Ltd., China). The impedance, transient photocurrent, and Mott-Schottky curves were determined by a model CHI660D electrochemical workstation (Shanghai Tatsuwa Instrumentation Co., Ltd., China).
The sample of 0.1 g was weighed and stirred in 100 mL of 20 mg/L MB solution, which was protected from light. For every 10 min, 3 mL of the sample was removed and the supernatant was centrifuged to determine the concentration of MB by a UV spectrophotometer. The adsorption performance was evaluated by a ratio of the concentration of the solution after adsorption, ct, to the initial concentration of MB, c0, at time t (ct/c0). After dark adsorption equilibrium, a 300 W xenon lamp was used as a light source, a filter (λ>420 nm) was added to simulate visible light, the distance from the light source to the liquid surface was fixed at 15 cm, the sample of 3 mL was taken for every 5 min, and the supernatant was centrifuged to determine the concentration of MB by a UV spectrophotometer. The photocatalytic performance was evaluated by a ratio of the concentration of the degraded solution to the initial concentration of MB, c0, at the time of t′ (ct/c0).
Five cycling experiments were performed on AG and SAG-1 to evaluate the stability of the photocatalytic properties of the materials. The stability of the crystal structure of the materials was evaluated based on the XRD patterns after each cycle.
Results and discussion The XRD patterns show that the introduction of SiO2 has no effect on the crystal structure of Ag10Si4O13. The TEM images of SAG-1 indicate the presence of graphene oxide, Ag10Si4O13 and SiO2. The UV-Vis diffuse reflectance spectra show that the edge of the absorption band of SAG-1 extended to 660 nm, which can be caused by the defects formed during the preparation of the material, but the forbidden bandwidth changes slightly, indicating that the protective layer of SiO2 does not cause any significant changes in the band gap. The PL spectra show that the fluorescence intensity of the material increases gradually with the increase in the content of amorphous SiO2, showing that the photogenerated carrier complexation rate increases with the increase of SiO2 incorporation. The photocatalytic performance of Ag10Si4O13 decreases significantly from 99% to about 90% after 5 cycles, while the photocatalytic performance of SAG-1 does not change after 5 cycles and still reaches 97%. The results show that the introduction of a small amount of SiO2 can slow down the reduction production of Ag+ during the photocatalytic degradation of Ag10Si4O13, and the crystal structure remains stable after some cycles, which greatly improves the stability of the material structure.
Conclusions SiO2/Ag10Si4O13/GO ternary composites with different SiO2 composite amounts were synthesized by a sol-gel method with GO and excess silica sol in an one-pot method. The complexing agent citric acid was used as a "bridge" to allow Ag10Si4O13 nanoparticles to grow uniformly on GO, and the excess silica sol was attached to the precursor surface, forming an amorphous SiO2 protective layer after heat treatment. The introduction of the amorphous SiO2 protective layer did not affect the crystal structure of Ag10Si4O13, which could extend the visible-light response range of the composite photocatalyst and significantly improve the adsorption performance for cationic dyes. However, SiO2 could reduce the migration rate of photogenerated carriers and accelerate the assembly of photogenerated electron-hole pairs, affecting the photocatalytic performance of the material. An appropriate amount of amorphous SiO2 protective layer could improve the photoreduction resistance and cycling stability of Ag10Si4O13 photocatalysts, while maintaining the original photocatalytic activity. The degradation rate of the SAG-1 sample was still 97% after 5 cycles, and the crystal structure remained stable after 5 cycles (I(132)/I(111) =1.16). This work could provide an reference for solving the problem that the materials of Ag-based efficient photocatalysts could be susceptible to photocorrosion during the photocatalytic process.
, authors=Cuixia LI, Bo YUAN, Xin ZHANG, Anhang WANG, Youyou ZHANG, Haize JIN, Zhizhong YANG, authorsList=Cuixia LI, Bo YUAN, Xin ZHANG, Anhang WANG, Youyou ZHANG, Haize JIN, Zhizhong YANG, authorCompany=null, correspAuthors=null, authorNote=
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2改性Ag
10Si
4O
13/氧化石墨烯光催化降解亚甲基蓝的稳定性及机理, columnId=1321897768759709821, journalTitle=硅酸盐学报, columnName=第14届无机非金属材料专题研讨会专题—研究论文, runingTitle=null, highlight=null, articleAbstract=
Ag10Si4O13因具备适配可见光响应的能带结构和促进光生载流子分离的内建电场而成为备受关注的新型光催化剂之一。但光催化使役过程中，Ag10Si4O13中Ag+易被光电子还原而累积Ag单质，影响光催化体系循环稳定性。氧化石墨烯（GO）能有效转移光生电子，而无定形SiO2可抑制离子扩散浸出，有望减缓Ag10Si4O13的光还原。本工作基于溶胶-凝胶体系制备不同无定形SiO2添加量的x% SiO2/Ag10Si4O13/GO（SAG）复合材料，探究无定形SiO2添加量对晶体结构、形貌及光电化学性能的影响机制；继而以亚甲基蓝（MB）为目标物研究无定形SiO2添加量对暗光吸附性能、可见光下光催化活性和循环降解稳定性的影响。结果表明：无定形SiO2的引入可大幅提升Ag10Si4O13/GO基底的抗光还原能力，拓宽光响应范围、提升对MB的吸附性能；但无定形SiO2会一定程度抑制光生载流子的迁移，加速光生电子-空穴对的复合，因此复合体系光催化降解效率随引入量SiO2增加呈现先增后降趋势，其中1%（质量分数）SiO2/Ag10Si4O13/GO（样品SAG-1）可见光条件下下40 min降解率可达99%并展现了良好的循环稳定性，5次循环之后材料晶体结构趋于稳定，降解率仍能达到97%。
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李翠霞（1972—），女，博士，副教授。
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李翠霞（1972—），女，博士，副教授。
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