Catalysts
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2022
·Vol. 12
·期 4
·378
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IF 4.501
Feng Jiang,Jiansha Gao,Di Lang
Photocatalytic studies on contaminant degradation in water suspension generally suggest that the degradation reaction mainly takes place on the surface of the photocatalysts rather than in the water phase. The mechanism of selective degradation is often difficult to distinguish concerning the contribution of adsorption and radical selectivity. This study is thus designed to investigate the roles of two types of hydroxyl radicals, adsorbed hydroxyl radical (·OHa) and free hydroxyl radical (·OHf), on the selective degradation of catechol (CT) and resorcinol (RE). CT and RE are significantly different in adsorption on a TiO2photocatalyst with a highly exposed {001} facet. CT can be selectively degraded by TiO2and was highly correlated with adsorption. Free radical quenching experiment results showed that the degradation of CT can be identified as the combined effect of both ·OHaand ·OHf, while the degradation of RE was mainly due to the ·OHf. Electron paramagnetic resonance coupled with spin trapping agents was used to detect the relative concentration of hydroxyl radicals in all the photocatalytic degradation processes. After a series analysis, we proposed that the mechanism of selective degradation mainly depends on the concentration of ·OHffor the pollutant molecules with weak adsorption on the catalyst surface.Keywords:photocatalytic;TiO2;catechol;resorcinol;hydroxyl radical;degradation selectivity
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Journal of Physical Chemistry C
·
2018
·
IF 4.484
Xing Xu,Lei Lai,Tao Zeng,Yan Yu,Zhiqiao He,Jianmeng Chen,Shuang Song
The exploration of low-cost, high-performance, and stable photocatalysts for the highly efficient conversion and storage of solar energy in hydrogen is of great importance. This study presents a novel pyridine-type carbonitrides (CN)-modified surface-disordered C-doped TiO2 (PCN/CTiO2@TiO2–x) catalyst used for photocatalytic H2 evolution from water. The employed preparation method of hydrolysis–calcination has the advantages of low-cost raw materials and easy scale-up. The optimized PCN/CTiO2@TiO2–x exhibited an impressive hydrogen evolution rate of ∼3743 μmol h–1 g–1 under simulated solar light (AM 1.5) and remained stable after five cycles. The maximal quantum efficiency reached 37.5% at 370 nm and 7.0% at 400 nm, which was superior or comparable to several reported relevant TiO2-based catalysts. Benefiting from the pyridine-type CN modification, disordered surface layer (TiO2–x), and increased oxygen vacancies/Ti3+ species, the photogenerated electrons moved rapidly from the visible-response C-doped TiO2 to CN to participate in the photoreduction reaction, which led to a marked improvement in the catalytic activity.
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CHEMOSPHERE
·
2015
·
IF 3.34
Qiong Tan,Guiqiu Chen,Guangming Zeng,Anwei Chen,Song Guan,Zhongwu Li,Yanan Zuo,Zhenzhen Huang,Zhi Guo
Immobilized Phanerochaete chrysosporium loaded with TiO 2 nanoparticles (PTNs) are novel high-value bioremediation materials for adsorbing cadmium and for degrading 2,4-dichlorophenol (2,4-DCP). The real-time changes in H + and O 2 fluxes were measured using the noninvasive microtest technique (NMT). The H + influx increased after the addition of 2,4-DCP, and shifted to efflux following the addition of Cd 2+ . The O 2 flux decreased after the addition of both 2,4-DCP and Cd 2+ . A larger Cd 2+ flux was immediately observed after exposure to 0.5 mM Cd 2+ (−351.25 pmol cm −2 s −1 ) than to 0.1 mM Cd 2+ (−107.47 pmol cm −2 s −1 ). The removal of Cd 2+ by the PTNs increased more after treatment with the 0.5 mM exposure solution (27.6 mg g −1 ) than with the 0.1 mM exposure solution (3.49 mg g −1 ). The enzyme activities were analyzed to review the antioxidative defense system of PTNs in a solution containing various concentrations of Cd 2+ . The activities of the coenzyme nicotinamide adenine dinucleotide (NADH) oxidase as well as the enzyme catalase (CAT) plateaued at 6.5 U g −1 FW and 9.7 U g −1 FW, respectively, after exposure to 0.25 mM Cd 2+ . The activity of superoxide dismutase (SOD) increased gradually in solutions containing 0.1–0.6 mM Cd 2+ , and eventually reached a maximum (68.86 U g −1 FW). These results illustrate how the antioxidative defense system and the physiological fluxes of PTNs respond to the stress caused by toxic pollutants .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Hu Wang,Bingxia Wu,Yuan Cai,Chengwei Zhou,Nengjie Feng,Geng Liu,Chong Chen,Hui Wan,Lei Wang,Guofeng Guan
The core–shell-structured Co–Z@TiO2(N2+O2) catalyst, which was prepared by subsequent pyrolysis and calcination from precursor ZIF-67 coated by amorphous TiO2, was applied in Fischer–Tropsch synthesis (FTS). Compared with Co–Z@TiO2 catalyst, which was directly calcinated in air (Co–Z@TiO2(O2)) or pyrolyzed in N2 (Co–Z@TiO2(N2)), the Co–Z@TiO2(N2+O2) catalyst showed better dispersion, easier reducibility, and optimal metal cobalt particle size (8.4 nm) due to the intermediate pyrolysis treatment and core–shell structure. The Co–Z@TiO2(N2+O2) catalyst exhibited high cobalt time yield (14.84 μmolCO·gCo–1·s–1), high selectivity to C5+ (81.5%), and low selectivity to low carbon hydrocarbon (CH4 (12.7%) and C2–C4 (5.8%)). The core–shell structure could enhance diffusion limitations to transform intermediate products into heavier hydrocarbons. After 110 h of evaluation, the Co–Z@TiO2(N2+O2) catalyst still maintained good catalytic performance and cobalt particle size distribution.
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CHEMOSPHERE
·
2021
·
IF 7.086
Hangjun Zhang,Yinan Zhang,Yuchi Zhong,Jiafeng Ding
Polychlorinated dibenzo-p-dioxins (PCDDs), characterized by their extreme toxicity, high persistency and bioaccumulation, regard as one of the most concerned environmental pollutants on the priority list. In this study, microwave-hydrothermal and photoreduction methods were adopted for fabrication of ternary Au@Fe/TiO 2 composites for removal of 2,8-dichlorodibenzo-p-dioxin (2,8-DCDD) under UV–Vis light irradiation. The acquired materials were characterized and analyzed by XRD, TEM, XPS, UV–Vis DRS, PL , etc. As a result, the 1%Au@1%Fe/TiO 2 exhibited much higher photocatalytic activity that 96.3% of 2,8-DCDD was removed within 160 min with respect to that of Fe/TiO 2 (3.0 times) and TiO 2 (5.5 times). It revealed the active substances might be produced, which were verified by ESR analysis. In a comparison, the 1%Au@1%Fe/TiO 2 also exhibited high activity in that 97.2% of 2,8-DCDD was removed within 240 min under an anoxic atmosphere. The 1%Au@1%Fe/TiO 2 systems were all pH-dependent that 2,8-DCDD could be fully degraded in neutral conditions. The results of repeatability on 1%Au@1%Fe/TiO 2 showed that the sample was high stability. Fe doping improved the charge separation of TiO 2 and Au modification improved the activity via SPR effect and Mott-Schottky barrier. The degradation mechanisms and pathways were proposed and discussed in detail. The current work develops a new approach on photocatalytic oxidation and reductive dechlorination of dioxins and may open a new opportunity to extend the application range of TiO 2 catalysts.
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Haoran Wang,Wei Ji,Feng Xiao,Yewen Xiao,Linlin Li,Xia Shu,Hualin Wang,Jun Yin
Over-ripening and spoilage of fruits, driven by excessive ethylene (C 2 H 4 ) production and microbial proliferation, present critical challenges in fruit postharvest preservation. Herein, a multifunctional photocatalytic film, CTC-Arg@CS/HPMC, is developed by incorporating chlorophyll-TiO 2 @carbon sphere (CTC) photocatalyst and L-arginine (Arg) NO donor into chitosan/hydroxypropyl methylcellulose (CS/HPMC) matrix for banana preservation. The distinctive dual heterojunction structure of CTC enhances photocatalytic activity under visible light, promoting reactive oxygen species (ROS) generation that triggers NO release from Arg. Under combined action of ROS and NO, CTC-Arg@CS/HPMC can not only inactivate bacteria with high antibacterial efficiency against Escherichia coli (93 ± 3 %) and Staphylococcus aureus (99 ± 2 %) within 60 min but also delay fruit ripening through C 2 H 4 degradation and inhibition of biosynthesis. In practical application scenario, CTC-Arg@CS/HPMC can effectively extend banana shelf-life by over 100 % at 25 °C, highlighting its potential as an active packaging material for extending the postharvest life of climacteric fruits.
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WATER RESEARCH
·
2022
·
IF 13.4
Cheng Hou,Xinbai Jiang,Dan Chen,Xiaoyu Zhang,Xiaodong Liu,Yang Mu,Jinyou Shen
Due to the pivotal role of Ag-TiO 2 /biofilm/nitrate interface, enhanced visible light-assisted biodegradation of tetracycline (TC) in anoxic system was realized through both batch experiment and long-term operation in this study. The results of the batch experiment elucidated that 50 mg L −1 TC could be completely removed within 10 h in Ag-TiO 2 /biofilm/nitrate system. The continuous flow experiment was operated for 75 d to evaluate the performance and stability of Ag-TiO 2 /biofilm/nitrate system. TC removal efficiency in Ag-TiO 2 /biofilm/nitrate system was as high as 92.4 ± 1.6% at influent TC concentration of 50 mg L −1 TC and hydraulic retention time (HRT) of 10 h, which would be attributed to the promoted separation of photoholes and photoelectrons at the presence of nitrate as electron acceptor. Facilitated electron transfer between semiconductor and biofilm was beneficial for enhancing TC biodegradation, thus lowering toxicity of intermediate products and promoting microbial activity. Moreover, the species related to TC biodegradation ( Rhodopseudomonas, Phreatobacter and Stenotrophomonas ), denitrification ( Thauera ) and electron transfer ( Delftia ) were enriched at Ag-TiO 2 /biofilm/nitrate interface. Besides, a possible mechanism involved in enhanced TC degradation and nitrogen removal at Ag-TiO 2 /biofilm/nitrate interface was proposed. This study provided a novel and promising strategy to enhance recalcitrant TC removal from industrial wastewater.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
IF 9.136
Zhengda Lin,Yijun Liu,Zhongming Zhang,Jie Yao
In this study we used a high-temperature steam-induced hydrolysis method to obtain a fluorinated OH/SiO 2 -TiO 2 /polyethersulfone (PES) composite hollow fiber membrane for CO 2 capture. The purpose of grafting SiO 2 and TiO 2 on the surface of PES by hydrolyzing silicon precursors and titanium precursors at high temperature, is to improve the alkali corrosion resistance and hydrophobicity of the PES membrane. The OH/SiO 2 -TiO 2 /PES composite hollow fiber membranes prepared by the high-temperature steam-induced hydrolysis method and the graft coating method were measured by SEM, EDS , FTIR, WCA, AFM , XRD and XPS in order to characterize the morphology and structure of the prepared membranes. In the CO 2 /CH 4 separation performance test experiment, the OH/SiO 2 -TiO 2 /PES membrane prepared by the high-temperature steam hydrolysis method showed better separation performance than the original PES membrane. The effects of absorbent flow rate, absorbent concentration and feed gas flow rate on CO 2 flux and CO 2 /CH 4 were selectivity investigated. When the flow rate of the absorbent (DEA) reached 16 L/h, the flow rate of the feed gas (CO 2 /CH 4 = 40 : 60) was 30 ml/min, the concentration of the absorbent was 1 mol/L, The CH 4 concentration was 99.88 % and the optimal separation factor was as high as 554.89. In general, the results obtained in this work may provide promising insights into the use of fluorinated OH/SiO 2 -TiO 2 /PES composite membranes for carbon capture and CO 2 /CH 4 separation in GLMC application.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 21
·6166-6179
·
IF 5.726
Qian Luo,Qi Zhou,Yan Lin,Shaohua Wu,Hongyu Liu,Cheng Du,Yuanyuan Zhong,Chunping Yang
The synthesis of high-performance and recyclable catalysts for oxidative desulfurization (ODS) from fuels has been a significant challenge. In this study, novel catalysts of MoO3–TiO2@MCM-22 with excellent catalytic performance were successfully prepared via a facile impregnation method. The results showed that the optimal catalyst at the Mo–Ti mass ratio of 1 : 4 (MT-1 : 4) exhibited highest catalytic efficiency for the ODS of dibenzothiophene (DBT) with a sulfur conversion of 99.96% within 15 min. Interestingly, the enhanced ODS activity was attributed to the synergistic effect between MoO3 and TiO2, which was achieved by adjusting the concentrations of Lewis and Brønsted acid sites on the surface of MCM-22. The catalyst MT-1 : 4 achieved the highest concentrations of Lewis and Brønsted acid sites and the largest combined index, resulting in the formation of peroxometallate complexes. Moreover, the kinetic studies revealed that the ODS was a pseudo first-order reaction with an apparent activation energy of 48.9 kJ mol−1. There was no significant reduction in the catalytic activity after 8 successive cycles, which manifested the perfect reusability of the catalyst MT-1 : 4 for the ODS system. Furthermore, a plausible ODS mechanism was proposed using the MoO3–TiO2@MCM-22 catalyst. Therefore, the prepared MoO3–TiO2@MCM-22 catalyst exhibited favorable industrial application potential for ODS.
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CERAMICS INTERNATIONAL
·
2024
·
IF 5.1
Zaizhi Yang,Xi Wang,Liang Zhang,Hailin Li,Hui Zhang,Dong Xu
(Ca, Ta) co-doped TiO 2 ceramics were successfully prepared using flash sintering technology, and the effects of oxygen vacancies on the rapid densification and giant dielectric properties were studied. The results suggest that the maximum volume fraction of oxygen vacancies in flash-sintered samples is approximately 10%. Oxygen vacancies decrease the barrier energy level of atomic diffusion and provide convenient diffusion channels, resulting in rapid densification of the sample within 24 min at 1100 °C. All flash-sintered samples exhibit high relative density, exceeding 95%. Oxygen vacancies promote the electron-pinning defect dipole effect at low temperatures. As the temperature increases, carriers such as oxygen vacancies move to the grain boundary, forming an internal barrier layer capacitance effect. The optical dielectric constant reaches 7.25 × 10 4 , and the dielectric loss drops to 0.09. Oxygen vacancy play an important role in both flash sintering technology and the giant dielectric properties of co-doped TiO 2 ceramics.
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Shibo Yu,Yiqing Zeng,Mengna Zhan,Shule Zhang,Zhaoxiang Zhong
The influence of phosphorus (P) on ammonia selective catalytic reduction (NH 3 -SCR) catalysts has been the subject of considerable scrutiny. Nevertheless, the precise mechanism of its influence remains a matter of contention. Furthermore, the impact of introducing P at varying stages during catalyst preparation process and its different sites within the catalyst structure on performance is frequently disregarded, significantly hindering practical guidance for designing effective modified catalysts. In this study, a series of P-modified CeO 2 /TiO 2 catalysts were synthesized by introducing P at different preparation stages, and various of characterization and comparison experiments were conducted to elucidate the effect of introducing P at different stages on NH 3 -SCR performance of NO x . Results show that introducing P before loading CeO 2 boosts catalyst activity, whereas delaying the introduction of P results in decreased activity and a progressive decline in catalyst performance as the sequence of P introduction is postponed. P introduced earlier tends to be distributed on the surface of the TiO 2 support, which contributes to the dispersion and anchoring of Ce species. In contrast, when the introduction of P was delayed, it tended to be distributed on the surface of the active species, which led to pore plugging and active sites being covered. Secondly, the variation in loading sites resulting from alterations in the stage of P introduction significantly affected on the chemical environment of Ce species, leading to notable differences in the redox capacity of the catalysts. This is the primary reason for the considerable discrepancy in the SCR performance of the catalysts. This study revealed the sensitivity of the stage of P introduction to CeO 2 /TiO 2 catalysts, providing new insights for designing modified CeO 2 /TiO 2 catalysts.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Cuicui Zhou,Shiqi Hong,Xinyu Chen,Quanfeng Li,Zongqi Chen,Songwang Yang
The electron transport layer (ETL) plays a critical role in efficient and stable perovskite solar cells (PSCs). The current effective method for the large-scale preparation of metal oxide ETLs is mainly based on expensive sputtering processes. Here, a screen-assisted self-spreading method is proposed as a novel approach to prepare uniformly thin and conformal TiO2 films on a rough fluorine-doped tin oxide (FTO) substrate as an ETL in planar PSCs. The TiO2 ETL deposited by this method exhibited good coverage and homogeneity on the rough FTO substrate, thereby minimizing interfacial recombination. The photovoltaic performance of the PSCs fabricated by this method is superior to that of the cells fabricated by spin coating, especially in terms of the fill factor. The performance enhancement can be attributed to the complete coverage of the FTO substrate by the conformal TiO2 film, confirming the effectiveness and reliability of the proposed method for the preparation of the TiO2 ETL. The advantages of this method lie in its scalability to prepare oxide films with a large area, eliminating the requirement of complex equipment, such as spinners, sputters, or physical vapor deposition equipment.
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