CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Zhijian Xiao,Wenda Yang,Jing Wang,Shuang Cao,Jingling Yang,Mingshan Zhu
Photocatalysis is a promising technology for removing low concentrations of nitric oxide (NO) from the atmosphere. However, the unsatisfactory photocatalytic NO removal efficiency and the high selectivity for NO 2 in catalysts limit the development of this technology. In this work, we used an in-situ synthesis method to incorporate Cs 3 Bi 2 Br 9 into UiO-66 for efficient and robust photocatalytic NO removal. The Cs 3 Bi 2 Br 9 /UiO-66 catalyst exhibits a 77.6 % NO removal efficiency and low NO 2 selectivity under visible light irradiation at a WHSV of 1,650,000 mL h −1 g −1 , exceeding the efficiencies of Cs 3 Bi 2 Br 9 (36.4 %) and UiO-66 (2.3 %), as well as those of most reported MOF-based photocatalysts. The synergy of weak Lewis acid sites from Cs 3 Bi 2 Br 9 in Cs 3 Bi 2 Br 9 /UiO-66 and the strong Lewis acid sites from UiO-66 promotes the enrichment of NO on the catalyst surface and act as electron traps to induce carrier separation, thereby promoting the generation of O 2 − to achieve high efficiency. This work provides a new idea for the development of catalysts in NO elimination.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Liangdong Hu,Lian-hua Xu,Chenjun Yang,Longfei Hong,Kai Wu,Sheng Chu,Longlong Ma,Shurong Wang,Rui Xiao,Huiyan Zhang
Lewis acid sites (LASs) are essential for the photocatalytic isomerization of biomass into high-value platform compounds. However, transient changes in the number of LASs in a photocatalytic system have not been clearly documented, often resulting in an inaccurate understanding of their role in isomerization. To address this challenge, in this study, the molecular probes glyceraldehyde was isomerized to 1,3-dihydroxyacetone (DHA, 63.5 % yield , 3 h) and fructose (47.9 % yield , 3 h) on Pt–KC 3 N 4 , with concurrent production of H 2 (233.8 μmol g −1 ). The results of in situ NH 3 –temperature-programmed desorption (TPD) characterization demonstrated that light irradiation induced the formation of transient LASs on Pt–KC 3 N 4 , and the density of acid sites observed in this study differed significantly from that observed in offline data. Furthermore, theoretical calculations demonstrated that photothermal electron redistribution on Pt–KC 3 N 4 is the main factor driving this transient LAS formation. This report describes a unique methodology to explore transient acid sites in isomerization reactions and provides insight into potential applications in the field of photocatalytic biomass valorization.
研究领域:
化学
·
可再生能源
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生物质转化
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DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2023
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IF 8.6
Weirui Chen,Muxin Lin,Jiaxin Zhou,Xukai Li,Xipeng Wei,Gaozu Liao,Jing Wang,Laisheng Li
Lewis acid site was vital center for activating O 3 during catalytic ozonation process. Herein, we proposed a strategy to enhance the Lewis acid strength of Fe-MCM-48 (FeM) by fluorination. Fluorinated Fe-MCM-48 (FFeM) exhibited the better catalytic ozonation efficiency towards Ketoprofen (KET), a kind of nonsteroidal anti-inflammatory drug. 87.4 % TOC removal was obtained by F 2.5 Fe 0.8 M/O 3 process, but only 27.5 % and 52.7 % were found by sole ozonation and Fe 0.8 M/O 3 processes, respectively. Comparative characterizations, experiments and DFT calculations showed that fluorinated FFeM was regular sphere with three dimensional duct channel and large S BET . Doping of F reduced particle size, implanted electron withdrawing Si-F group and formed the electron poor center around Fe atom, which enhanced Lewis acid strength of FFeM. Protonated hydroxyl groups on Lewis acid sites were the main active sites for O 3 activation. Greater amount of O 3 were absorbed on the surface of FFeM and the greater O 3 utilization rate, •OH and •O 2 – generation rates were obtained by FFeM/O 3 process. Common anions such as Cl − , SO 4 2− and NO 3 – and Humic acids (HA) had little effect on KET removal but inhibited TOC removal in FFeM/O 3 process. •OH, •O 2 – and Fe(IV) = O oxidation were accounted for KET degradation. 16 kinds of intermediates generated from KET degradation and 4 pathways were deduced.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Jialing Shen,Guojun Lv,Juan Deng,Shihao Su,Fuxin Wang,Shengnan Xu,Lachgar Oussama,Zhongmin Liu
UiO-66 materials have the benefit of excellent stability, porosity, huge surface area, and presence of flaws, hence designing oxidative desulfurization (ODS) catalysts based on UiO-66 is very appealing. Herein, tungsten doped UiO-66 materials were synthesized with post-doping and in situ synthesis methods, and used as heterogeneous catalysts for the room-temperature oxidative desulfurization reactions. The successful doping of tungsten into the UiO-66 framework was demonstrated by FT-IR, UV–Vis, Raman and TGA characterizations. XAS characterization disclosed that tungsten element formed Zr-O-W bond on the defect sites for the tungsten doped UiO-66 materials. At the same time, the in situ synthesized W 2 @U-150 catalyst revealed the highest 98.5% of dibenzothiophene (DBT) elimination within 1h of desulfurization reaction as well as the biggest catalytic efficiency of 17727.3 h −1 mol −1 at room temperature due to its smallest band gap energy of 3.32 eV, highest tungsten content of 9.8 %, and most Lewis acid amount of 47.1 μmol/g. In addition, the synthesized W 2 @U-150 catalyst showed excellent re-usability for five cycles.
研究领域:
材料科学
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催化化学
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环境化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 22
·6561-6569
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IF 5
Songlei Mo,Yong Guo,Xiaohui Liu,Yanqin Wang
The glycolysis of polyethylene terephthalate (PET) is considered as the most promising PET recycling strategy due to its mild reaction conditions and circularity. Herein, several metal-doped SBA-15 (M/SBA-15) as heterogeneous Lewis acid catalysts were investigated to screen the best catalyst and to understand the essence for their differences in PET glycolysis. It is found that the catalytic activity is positively correlated with the acid amount in different metal-doped SBA-15 and Ti/SBA-15 with different Ti loadings, with the exception of Nb/SBA-15. 4Ti/SBA-15 with abundant Lewis acid sites shows excellent PET glycolysis ability, with the yield of bis(2-hydroxyethyl) terephthalate (BHET) reaching 87.2% within 45 min at 190 °C (isolated yield 73%). While 4Nb/SBA-15 has a similar acid amount as that in 4Ti/SBA-15, but it has very low catalytic activity probably due to its strong oxygen affinity. Acetone–methanol-adsorption DRIFTS confirms its strong oxygen affinity, which would poison the acid sites by ethylene glycol (EG) and result in very low activity. This study demonstrates that PET glycolysis activity is really correlated with the amount of Lewis acid sites, but species with very strong oxygen affinity would lower its activity. Further diffuse reflection ultraviolet-visible (DR UV-vis) spectra analysis confirms that tetrahedral Ti4+ species in Ti/SBA-15 is the real active center. In addition, 4Ti/SBA-15 has good reusability and can be used in common real PET (dyed polyester fabric, PET bottles) glycolysis. These results indicate that increasing the amount of Lewis acid sites is a promising way to enhance PET glycolysis and 4Ti/SBA-15 with high activity and stability is a potential catalyst for industrial application.
研究领域:
材料科学
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催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2015
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IF 3.352
Hui-Ying Sun,Lin-Ping Sun,Fei Li,Long Zhang
The adsorption of benzothiophene from fuels on NaY zeolites modified with 0.09 M NaOH aqueous solution was investigated. The sulfur removal reached to 99.9%, and the adsorption capacity was 1.65 mg benzothiophene/g of the modified adsorbent. The results of the scanning electron microscopy, X-ray diffraction, X-ray fluorescence, and N 2 adsorption–desorption isotherms analyses show that mesopores appeared on the surface of NaY-0.09 adsorbent and the intrinsic crystallinity was preserved after the modification. Py-IR and NH 3 -TPD analyses indicated that the adsorption of benzothiophene occurred on the weak Lewis acid sites on the adsorbent. Both an increase in the number of the weak Lewis acid sites and the formation of mesopores on NaY-0.09 adsorbent improved its desulfurization activity.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
Cell Reports Physical Science
·
2022
·
IF 7.832
Xingmei Lu,Jingkun Yu,Jinmeng Cai,Qinghua Zhang,Siwei Yang,Lin Gu,Geoffrey I.N. Waterhouse,Shuang-Quan Zang,Bai Yang,Siyu Lu
Electrocatalytic nitrate reduction represents a very promising route for ammonia synthesis under ambient conditions. However, for most nitrate-to-ammonia electrocatalysts developed to date, the Faradaic efficiency (FE) to ammonia is modest due to the competitive hydrogen evolution reaction (HER). Here, we report that the decoration of vertically aligned NiCo 2 O 4 pillars with boron-doped carbon dots (BCDs) enables electrocatalytic nitrate reduction to ammonia with ∼100% FE. A BCDs/NiCo 2 O 4 /carbon cloth cathode delivers a NH 3 production rate of 173.9 μmol h −1 cm −2 at −0.55 V versus reversible hydrogen electrode (RHE). This state-of-the-art performance is linked to the BCDs, which provide an abundance of Lewis acid sites on the electrocatalyst surface for the adsorption of nitrate ions (simultaneously suppressing the competitive HER). This work reveals that highly selective NH 3 electrosynthesis can be achieved under ambient conditions by regulating the surface acidity/basicity properties of metal-oxide-based catalysts, paving the way toward more sustainable NH 3 -production technologies.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Jian Wang,Yueyang Xu,Erjian Huang,Liming Kong,Jie Li,Yongping Zeng
The combustion of thiophene sulfides in fuel leads to the release of sulfur oxides (SO x ), which pose significant threats to both ecological systems and human health. Adsorption desulfurization has gained considerable attention from researchers due to its mild operating conditions, low production costs, and minimal impact on octane number. This study investigates the use of Cu-BTC as a platform for developing a novel adsorbent aimed at efficiently removing thiophenic compounds from fuel. Aluminum atoms were incorporated into the framework of Cu-BTC to create micro/mesoporous Al/Cu-BTC. Subsequently, the π-complexation adsorbent Al/Cu(I)-BTC, featuring Lewis acid sites, was synthesized through the in-situ reduction of Al/Cu-BTC using sodium thiosulfate. The adsorption properties of Al/Cu(I)-BTC for thiophene were assessed through both batch and breakthrough experiments. Al/Cu(I)-BTC-0.10(0.28) demonstrated exceptional adsorption performance. The static and dynamic adsorption capacities of thiophene at 500 and 200 ppm were 18.54 mg S/g and 9.49 mg S/g, respectively. Importantly, the adsorption capacity of Al/Cu(I)-BTC-0.10 (0.28) for thiophene in fuel containing 500 ppm sulfur remained at 15.45 mg S/g after six regeneration cycles. In the competitive adsorption of toluene, the adsorption capacity of the adsorbent for thiophene in the fuel containing 200 ppm sulfur was 7.84 mg S/g.
研究领域:
材料科学
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环境科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Pingping Wu,Lei Song,Yue Wang,Xuehua Liu,Zhengke He,Peng Bai,Zifeng Yan
Achieving the balance between the catalytic activity and product selectivity still remains a challenge in partial oxidation processes, because the products are prone to be over-oxidized. Lewis acids (such as AlCl 3 ) have previously been identified to interact with C O groups, which can prevent the ketone products from further transformation. In this work, ZrO 2 promoted Au-Pd/γ-Al 2 O 3 catalyst was designed to enhance the benzaldehyde selectivity by generating more surface Lewis acid site on ZrO 2 -modified alumina. Results show that the introduction of ZrO 2 (5%) resulted in the formation of more surface Lewis acid sites, which improved the benzaldehyde selectivity through the strengthened interaction between the Lewis acid sites and C O groups in benzaldehyde. Besides, the addition of small amount of ZrO 2 enhanced the noble metal dispersion and led to the formation of more active sites to improve the oxygen transfer during the reaction.
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
Small
·
2024
·
IF 13
Yangyang Ren,Beibei Li,Guichao Zhang,Zunming Lu,Lanlan Li,Xiaojing Yang,Xinghua Zhang,Xiaofei Yu
Improvement in the durable and active low-Pt nanocatalysts for oxygen reduction reaction (ORR) is the essential target for clean energy. Herein, an efficient CeO 2 supported PtCu alloy catalyst (PtCu/CeO 2 -C) for ORR in acid media is developed. The CeO 2 support can effectively anchor the PtCu particles and inhibit their migration during the long-life cycling, which is beneficial to the catalytic performance. According to the electrochemical experiments, the specific and mass activities of PtCu/CeO 2 -C are 1.09 mA cm −2 and 0.49 A mg Pt −1 at 0.9 V, which are 9.9 and 6.1 times as large as that of Pt/C, demonstrating its outstanding ORR activities in acid media. Moreover, the theoretical studies confirm that oxygen vacancies (V O ) as Lewis acid sites can facilitate the adsorption and dissociation of O 2 , regulate the electronic structure of Pt, and thus endow PtCu/CeO 2 -C with an efficient 4-electron ORR pathway. The results suggest that the rational design of supported Pt-based catalysts is of great significance for efficient ORR reaction.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Zijun Huang,Yubing Li,Yongming Luo,Dingkai Chen,Xiaohua Cao,Hao Wang,Shuquan Huang,Dedong He
The distribution and location of active metal in zeolite determine the performance in catalytic processes, and catalysts encapsulated with small-sized and highly dispersed metal sites have received tremendous progress in propane dehydrogenation (PDH), while the identification of the migration of metal sites in silicalite-1 (S-1) and its structural characteristics have been rarely investigated. In this work, we engineered the location of cobalt in the S-1 by developing dissolution and recrystallization method, and migration behavior of cobalt during recrystallization stage is systematically investigated. It is found that active Co 2+ species are mainly located at the intersection of straight and sinusoidal β channels, and the abundance of Co 2+ located at β channel increase Lewis acid site of the catalyst, which regulates the catalyst more active in the PDH process. This work enriches a deep understanding of the β-located Co 2+ sites, and provides a novel idea for the synthesis of high-performance PDH catalysts.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2017
·
IF 4.601
Xiaotian Zhang,Pengcheng Huang,Aili Liu,Mingyuan Zhu
Owing to the high prices and other shortcomings associated with the existing methods of complex catalyst preparation, we used the UIO-66(Zr) metal–organic frameworks to directly catalyze the oxidative desulfurization (ODS) reaction. The synthesized UIO-66(Zr) was characterized using nitrogen adsorption–desorption isotherm analysis, X-ray diffraction, Fourier transform infrared spectroscopy, transmission electron microscopy, and X-ray photoelectron spectroscopy. Under optimal reaction conditions, the ODS conversion of dibenzothiophene (DBT) reached 100%. This excellent catalytic activity was attributed to the unsaturated coordination of Zr, which may produce beneficial Lewis acid sites.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）