DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 35
·12244-12252
·
IF 4
Shen Yu,Zhan Liu,Jia-Min Lyu,Chun-Mu Guo,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Ming-Hui Sun,Li-Hua Chen,Bao-Lian Su
The catalytic oxidative desulfurization (ODS) technique is able to remove sulfur compounds from fuels, conducive to achieving deep desulfurization for the good of the ecological environment. Ti-based metal–organic frameworks (Ti-MOFs) possessing good affinity to organic reactants and considerable numbers of Ti active sites are promising catalysts for ODS. However, current Ti-MOFs suffer from severe diffusion limitations caused by the size mismatch between sole micropores and bulky sulfur compounds, leading to poor ODS performance. Here, a facile method of intraparticle ripening without any additive is developed to obtain hierarchically meso–microporous Ti-MIL-125 single crystals (Meso-Ti-MIL-125) for the first time. Such Meso-Ti-MIL-125 shows a BET surface area of 1401 m2 g−1 and a mesoporous volume that is 1.7 times as high as that of the conventional Ti-MIL-125. Our novel Meso-Ti-MIL-125 exhibits excellent catalytic performance in the ODS of a series of bulky thiophenic sulfur compounds, completely removing benzothiophene (BT), dibenzothiophene (DBT), and 4,6-dimethyldibenzothiophene (DMDBT) from model fuels, which is, respectively, 2.4 times, 1.5 times, and 6.7 times higher than the removal achieved with conventional Ti-MIL-125. Such a facile synthetic strategy is envisioned to be applied in many kinds of crystalline materials, such as zeolites, for industrial production.
研究领域:
化学工程
·
材料科学
·
环境科学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Wen Xu,Xiaoshu Wang,Weilong Hou,Kang Tang,Xinqing Lu,Yijing Gao,Rui Ma,Yanghe Fu,Weidong Zhu
Although the titanosilicate zeolite catalyzed one-pot oxidative hydration of ethylene with hydrogen peroxide (H 2 O 2 ) to ethylene glycol (EG) takes advantages of step-saving and facile operation, both H 2 O 2 utilization efficiency and EG yield are relatively low. In the present work, Sn-doped Ti-MWW zeolites, named Sn-Ti-MWW, were developed for this oxidative hydration, showing the much higher H 2 O 2 utilization efficiency and EG yield, compared to Ti-MWW. The extensive characterizations of Sn-Ti-MWW zeolites, in combination with Density Functional Theory (DFT) calculations, verify that the doping of Sn into Ti-MWW leads to the higher electropositivity of the Ti species, resulting in the stronger acidity of the zeolite, which is helpful to the H 2 O 2 utilization and EG production. In addition, although the catalyst deactivation is observed due to the deposition of the bulky byproducts onto the active sites and/or into the zeolite micropores, the simple calcination of the used catalyst readily restores its catalytic activity. Therefore, it is anticipated that the developed Sn-Ti-MWW catalyst might be applicable in the one-pot oxidative hydration of ethylene with H 2 O 2 to EG industrially.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
Materials Today Communications
·
2024
·
IF 3.7
Xinbo Zhao,Zan Li,Yuye Dou,Xiaohui Jiang,Fan Bu,Zhenxia Liu,Liangmin Yu
Antibiotic wastewater poses a significant threat to the global environment and human health. In this work, Ni-Ti bimetallic Metal-Organic Frameworks (NT-MOF) were synthesized as effective photocatalysts to remove tetracycline (TC) from water under visible light irradiation. The photocatalysts underwent characterization using techniques such as Scanning Electron Microscopy (SEM), Transmission Electron Microscopy (TEM), X-Ray Diffraction (XRD), Fourier Transform Infrared Spectroscopy (FT-IR), N 2 adsorption-desorption, and X-Ray Photoelectron Spectroscopy (XPS). Photocatalytic tests were conducted under visible light conditions (λ>420 nm). The enhanced performance is mainly due to the presence of Ni in NT-MOF changing the shape and structure of the samples, reducing electron-hole recombination, thus promoting the charge separation process. These findings have significant implications for the development of efficient and sustainable methods for the removal of TC from wastewater.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscience and Nanotechnology Letters
·
2017
·Vol. 9
·期 9
·1356-1362
·
IF 1.889
Xu Jianxiong,Xie Shaowen,Feng Yahui,Du Jingjing,Xu Lijian
TiO2 nanoparticles with average diameter of 510 nm were prepared by sol–gel surfactants, and the hierarchically nanoporous Ti–SiO2 particles were further prepared using in-situ method. The hierarchically nanoporous Ti–SiO2 particles
with hollow structure were analyzed by transmission electron microscope (TEM), energy dispersive spectrometer (EDS), scanning electron microscope (SEM), nitrogen adsorption stripping curves and Barrett-Joyner-Halenda (BJH) pore size distribution curves. Finally, the hierarchically nanoporous
Ni–Mo composite electrodes were prepared using the TiO2 nanoparticles or nanoporous Ti–SiO2 particles as composite particles respectively, and the influence of the concentration of composite particles on the electrocatalytic activities of Ni–Mo composite
electrodes for hydrogen evolution were investigated by polarization curves. The results showed that the diameter of Ti–SiO2 particles was from 200 nm to 500 nm, and specific surface area was 573 m2/g with pore volume of 1.19 cm3/g and mesopore size of
3.2 nm. The TiO2/Ni–Mo and Ti–SiO2/Ni–Mo composite electrodes were fabricated by electrodeposition with TiO2 nanoparticles and nanoporous Ti–SiO2 particles as composite particles respectively. The electrocatalytic activities
of TiO2/Ni–Mo and Ti–SiO2/Ni–Mo composite electrodes for hydrogen evolution were investigated. Results showed that the electrocatalytic activities of TiO2/Ni–Mo and Ti–SiO2/Ni–Mo composite electrodes for hydrogen
evolution reached the optimal value when the concentration of particles was 4 g/L and 2 g/L respectively. The electrocatalytic activities of TiO2/Ni–Mo and Ti–SiO2/Ni–Mo composite electrodes were greater than that of Ni–Mo alloy electrode, and
the Ti–SiO2/Ni–Mo composite electrode showed the best electrocatalytic activity.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Wei Song,Hanqing Zhao,Jianqi Ye,Mengmeng Kang,Siyu Miao,Zhong Li
Ti–O–C channels for ultrafast sodium storage were constructed in N/S-co-doped TiO2–C nanofibers, which deliver a high rate performance of 181.9 mAh g–1 at 5 A g–1 after 3000 cycles. The existence of Ti–O–C bonds at the interface of TiO2–C phases was revealed by synchrotron radiation X-ray absorption spectra. Based on this, first-principles calculations further verified the low energy barrier for Na+ insertion/extraction in the Ti–O–C channels formed by the intimately integrated graphite layer with TiO2 near the surface. In addition, surface defects induced by heteroatoms accelerate the Na+ mass transfer through the pathway from the carbon surface to the Ti–O–C channel.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Wen Gao,Fangyuan Wang,Meilin Ou,Qianqian Wu,Lei Wang,Haonan Zhu,Yuanyuan Li,Ning Kong,Jianping Qiu,Shanshan Hu,Shuang Song
The presence of elevated levels of norfloxacin (NOR) in the aquatic environment presents a serious risk to both human health and environmental organisms due to its extremely toxic and persistent characteristics. Herein, a series of Fe/Ti bimetallic composites (NH 2 -MIL-53(Fe/Ti)) were prepared using a one-step hydrothermal method to assess their capability for NOR degradation and investigate degradation mechanisms. It was observed that the well-organized nanosheets interconnected to form chrysanthemum clusters contained a significant number of exposed edges and open pores, which facilitated the enrichment of NOR. Notably, the optimum NH 2 -MIL-53(Fe/Ti) (1.5:1) demonstrated excellent degradation performance for NOR under visible light, owing to an electronic interaction between Fe 3+ and Ti 4+ metal centers. Efficient NOR degradation by NH 2 -MIL-53(Fe/Ti) (1.5:1) was achieved at 84.6% after 120 min of irradiation. Furthermore, the NH 2 -MIL-53(Fe/Ti) (1.5:1) maintained excellent reusability and stability even after five cycles tests. Active species trapping experiments confirmed that the pivotal role of •O 2 − and h + in photodegradation of NOR pollutants. A plausible photocatalytic mechanism was suggested according to various performance characterization and experimental results. Defluorination and ring opening were the main degradation pathways. This work advanced our understanding of photogenerated carriers transfer and energy conversion in bimetallic MOFs . Additionally, a novel strategy was presented for visible light catalytic degradation of NOR, which were highly relevant for the field of environmental treatment.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2024
·Vol. 14
·期 8
·5142-5148
·
IF 3.9
Chunhong Jin,Jingchao Liu,Yilin Yin,Zenghe Li
In wastewater containing heavy metals, Cr(VI) is a potentially toxic metal, mainly derived from production and processing processes such as textile printing, dyeing, ore mining, battery applications, metal cleaning and electroplating. WO3 is widely used in photocatalytic degradation and reduction, and its utilization rate of visible light is high. However, the rapid recombination of photogenerated electron–hole pairs of WO3 limits its use. In this work, the composite material (WxMy) of WO3 and MIL-125 (Ti) was prepared by the ball milling method, and the catalyst was used to photocatalytically reduce Cr(VI). After using W90M10 as a photocatalyst for 50 min, the reduction rate of Cr(VI) can reach 99.2%, and the reduction rate is 2.3 times that of WO3. After 5 cycles of use, the reduction rate can still reach 91.3%. It is mainly due to the formation of a II-type heterojunction between WO3 and MIL-125 (Ti), which promotes the separation of photogenerated electron–hole pairs, thus improving the efficiency of photocatalytic reduction of Cr(VI).
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2022
·
IF 8.431
Yong Cheng,Han-Qing Zhao,Aqiang Ding,Fei Chen,Jun Liu,Dazhi Fang,Chenglong Li,Yongkui Huang,Peili Lu
The widespread application of quaternary ammonium compounds (QAC) has posed a serious hazard to the environment and human being, and high concentration of Cl − in QAC wastewater may further increase the difficulty of pollutants elimination . In this study, such a QAC wastewater under high salinity conditions was chosen as the target, the prepared Ti/(Ru x Ir y )O 2 anode exhibited favorable catalytic performance for the oxidation and mineralization of QAC under high salinity conditions. Increasing the Ru/Ir ratio of Ti-based electrode coating also slightly promoted the inner catalytic capacity. The combination of electron paramagnetic resonance (EPR) and quenching experiments indicates that 1 O 2 served as a main reactive specie in the Ti/(Ru x Ir y )O 2 electrooxidation system. The increase of pH could decrease the removal efficiency of QAC for the reduced 1 O 2 yield, and the rise of Cl − concentration could favor the QAC oxidation, and Cl − was a better electrolyte to promote the oxidation of organic contaminants when compared to Na 2 SO 4 or Na 2 CO 3 . Additionally, the conversion pathway of the model pollutant was tentatively investigated, the results demonstrated that there were almost no halogenated final products residual by electrocatalytic oxidation with Ti/(Ru x Ir y )O 2 anode. This study not only elucidate the reaction mechanism of Ti/(Ru x Ir y )O 2 anode electrocatalytic oxidation of high salinity QAC wastewater, but also may provide an efficacious and eco-friendly method for the treatment of high salinity QAC wastewater.
研究领域:
环境科学
·
污水处理
✓ 已验证
产品关联
DOI
PubMed
高影响因子
npj Quantum Materials
·
2022
·Vol. 7
·期 1
·1-8
·
IF 6.856
Zhang Wenhao,Gao Jingjing,Cheng Li,Bu Kunliang,Wu Zongxiu,Fei Ying,Zheng Yuan,Wang Li,Li Fangsen,Luo Xuan,Liu Zheng,Sun Yuping,Yin Yi
The electronic evolution of doped Mott insulators has been extensively studied for decades in search of exotic physical phases. The proposed Mott insulator 1 T -TaS 2 provides an intriguing platform to study the electronic evolution via doping. Here we apply scanning tunneling microscopy (STM) to study the evolution in Ti-doped 1 T -TaS 2 at different doping levels. The doping Ti atom locally perturbs the electronic and spin state inside the doped star of David and induces a clover-shaped orbital texture at low-doping levels ( x < 0.01). The insulator to metal transition occurs around a critical point x = 0.01, in which small metallic and large insulating domains coexist. The clover-shaped orbital texture emerges at a broader energy range, revealing a competition with the electron correlation. It transforms to a disorder-induced Anderson insulating behavior as doping increases. We directly visualize the trapped electrons in d I / d V conductance maps. The comprehensive study of the series of Ti-doped 1 T -TaS 2 deepens our understanding of the electronic state evolution in a doped strong-correlated system.
研究领域:
凝聚态物理
·
材料科学
·
表面科学
·
电子结构
·
量子材料
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2012
·
IF 2.103
Zhen Wang,Xinbo Ci,Hongjun Dai,Lu Yin,Huixiang Shi
A highly photoactive Ti-containing Cr-modified MCM-48 photocatalyst (Si/Ti = 3.4, Si/Cr = 50) was prepared by a facile one-step method at room temperature. A combination of various physicochemical techniques such as X-ray diffraction (XRD), N 2 physisorption, diffuse reflectance UV–vis spectra (DRS) and X-ray photoelectron spectra (XPS) were used to characterize the properties of the synthetic catalysts. The characterization and experimental results indicated that tetrahedral Ti oxide moieties as dominant Ti oxide were loaded into the mesoporous structure and there was a synergistic interaction between the Ti species anchored on the walls and the Cr ions presented in the MCM-48 framework, which was considered to be directly correlated to the photoactivity. The Ti-Cr-MCM-48 sample can remove H 2 S with the efficiency of 92% under visible light, being the Cr 6+ species primarily responsible for this photoactivity. A deactivation was observed as a consequence of sulfate accumulation on the surface of the catalyst and reduction of Cr 6+ .
研究领域:
材料科学
·
环境科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Mazhar Khan,Zeeshan Akmal,Muhammad Tayyab,Seemal Mansoor,Dongni Liu,Ziwei Ye,Jinlong Zhang,Shiqun Wu,Lingzhi Wang
The rational design of heterojunction photocatalysts is crucial for enhancing CO 2 photoreduction efficiency, yet precisely channeling photogenerated electrons to the CO 2 adsorption sites remains an enormous challenge. In this work, we developed an organic-inorganic heterostructure with continuous inter- and intra-component electric fields. The integration of BiOBr with MIL-125 via chemical bonding established a heterojunction, where the built-in electric field between the two components facilitated the efficient transfer of photogenerated electrons from BiOBr to MIL-125. The intrinsic electric field of MIL-125 further drove the accumulation of photogenerated electrons at Ti sites. This tandem electric field effect, in conjunction with the CO 2 adsorption and activation at Ti sites, significantly enhanced the efficiency of CO 2 reduction within the heterojunction system. The optimized photocatalyst achieving CO production at a rate of 65.6 μmol g −1 h −1 with nearly 90 % selectivity without the use of sacrificial agents, exhibiting a remarkable 43-fold and 8-fold enhancement in activity compared to pristine MIL-125 and BiOBr, respectively. In-situ infrared spectroscopy and theoretical calculations confirmed the energy optimization effect of the heterostructure on CO 2 activation and the hydrogenation reaction, facilitating the formation of the key intermediate *COOH. This work elucidates the mechanism by which tandem built-in electric fields facilitate charge separation.
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2024
·
IF 3.7
Yuanzhen He,Dengjie Zhong,Yunlan Xu,Ran Jiang,Jiayou Zhang,Pengfei Liao
A La-doped Ti/SnO2-Sb2O4 electrode with TiO2-NTs intermediate layer (Ti/TiO2-NTs/SnO2-Sb2O4-La) was created via the electrodeposition technique. The physicochemical and electrochemical properties of the electrode were analyzed through FESEM, XRD, XPS, CV, and LSV electrochemical tests. The results showed that TiO2-NTs were tightly packed on the surface of Ti substrate, thus improving the binding force of the SnO2-Sb2O4-La coating, offering greater specific surface area, more active spots, higher current response, and longer lifespan for the degradation of rhodamine B. The lifespan of the Ti/TiO2-NTs/SnO2-Sb2O4-La electrode reached 200 min (1000 mA cm–2, 1 M H2SO4), while the actual service life was up to 3699 h. Under the conditions of initial pH 3.0, Na2SO4 concentration of 0.1 M, current density of 30 mA cm–2, and initial rhodamine B concentration of 20 mg L–1, the color and TOC removal rate of rhodamine B reached 100% and 86.13% within 15 and 30 min, respectively. Rhodamine B was decomposed into acids, esters, and other molecular compounds under the action of •OH and SO4•– free radicals and electrocatalysis, and finally completely mineralized into CO2 and H2O. It is anticipated that this work will yield a novel research concept for producing DSA electrodes with superior catalytic efficacy and elevated stability.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）