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CATALYSIS COMMUNICATIONS · 2017 · IF 3.33

Atomic layer deposition of aluminium on anatase: A solid acid catalyst with remarkable performances for alcohol dehydration

Yingji Song,Shaodan Xu,Fei Ling,Panpan Tian,Tao Ye,Deqing Yu,Xuefeng Chu,Yingzi Lin,Xiaotian Yang,Junhong Tang

Here we reported the synthesis of Al sites with ultra-high dispersion on anatase by an atomic layer deposition (ALD) method (ALD-Al/TiO 2 ), which exhibits Brønsted acidity and satisfactory activity in the dehydration of alcohols, a key step in the deoxygenation of biomass. More importantly, the ALD-Al/TiO 2 catalyst has good stability, which is sintering-resistant and gives constant catalytic performances after treatments at high temperature.

研究领域: 化学工程 · 催化科学
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2020 · IF 16.683

Importance of controllable Al sites in CHA framework by crystallization pathways for NH3-SCR reaction

Juan Zhang,Yulong Shan,Ling Zhang,Jinpeng Du,Hong He,Shichao Han,Chi Lei,Sen Wang,Weibin Fan,Zhaochi Feng,Xiaolong Liu,Xiangju Meng,Feng-Shou Xiao

As a commerical catalyst of high silica CHA zeolite for NH 3 -SCR reaction, controllable Al sites in CHA framework for improving catalytic performance are rarely reported. In this work, two organic templates (TMAda + and DMCHA + ) were employed to prepare aluminosilicate CHA zeolite with similar Si/Al ratios, donated as CHA-T and CHA-D. Detailed characterizations demonstrate that two completely distinguishable crystallization pathways can be identified as the preferential formation of smaller D6R units for CHA-D with DMCHA + and larger 8MRs for CHA-T with TMAda + , resulting in spatially closer Al sites in CHA-D than CHA-T. As an interpretation, CHA-D with more paired Al atoms in 6MR generating more hydrothermally stable Cu 2+ -2Z sites contributes to higher activity than CHA-T at 400−550 °C. These results suggest that the crystallization pathways directed by rational choice of organic templates might be responsible for the controllable Al sites in the framework, which is important for designing efficient NH 3 -SCR catalysts.

研究领域: 材料科学 · 催化化学
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Catalysis Science & Technology · 2024 ·Vol. 14 ·期 14 ·4058-4067 · IF 4.4

Constructing tri-coordinated Al (AlIII) sites to boost complete propane oxidation of the Pt/Al2O3 catalyst

Yang You,Aijie Xu,Yao Lv,Lide Yang,Xuan Tang,Jie Tang,Yanglong Guo,Yao Cui,Wangcheng Zhan,Li Wang,Yun Guo,Sheng Dai

Complete oxidation of propane has drawn great attention in the fields of automotive emission control and volatile organic compound elimination. However, it is challenging to achieve high activity of this reaction due to the stability of propane. We here utilize a facile solvothermal method to construct tri-coordinated Al (AlIII) sites on the as-synthesized ST-Al2O3 support to alter the properties of supported Pt species. It is demonstrated that AlIII sites facilitate the dispersion and electron enrichment of supported Pt sites. Thus, Pt/ST-Al2O3 exhibits a superior activity toward complete propane oxidation, showing a 6.7-fold improvement in the turnover frequency over commercial Pt/Al2O3 catalysts. Meanwhile, Pt/ST-Al2O3 possesses a distinct reaction route originating from its stronger C–H and C–C cleavage capability, while having excellent activity not only in complete propane oxidation but also in the complete oxidation of other alkanes (CH4, C2H6, and n-C4H10). In addition, the AlIII construction strategy is successfully extended to more cases, e.g., Pd/ST-Al2O3 with higher Pd dispersion and electron density. This work provides a promising strategy for the control of the oxide support for advanced design and synthesis of alkane oxidation catalysts.

研究领域: 催化化学 · 环境科学 · 材料科学
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ACS Nano · 2024 · IF 15.8

Mineral-Mediated Epitaxial Growth of CoO Nanoparticles for Efficient Electrochemical H2O2 Activation

Guoqiang Zhao,Xiaoyu Tao,Tongsen Guo,Liangjie Fu,Huaming Yang

Solution-phase epitaxy is a versatile method to synthesize functional nanomaterials with customized properties, where supports play a central role as they not only serve as nucleation templates but also greatly affect the local electronic structures. However, developing functional supports remains a great challenge. Herein, inspired by the commonly observed epitaxy of minerals in the natural environment, we report using calcination-modified kaolinite as the support for the epitaxial growth of hexagonal CoO nanoparticles (h-CoO NPs), which enables over 40 times higher mass-specific activity toward H2O2 electrochemical activation than the counterpart without the support. High-resolution electron microscopy, magic-angle spinning nuclear magnetic resonance, and X-ray absorption fine structure results prove that the Al sites in kaolinite play a crucial role in the formation of h-CoO NPs. Moreover, the five-coordinate Al (AlV) sites produced by the dehydration of kaolinite are indispensable for forming the epitaxial interface. Theoretical calculations reveal that the local electron densities around AlV sites are lower than those of general six-coordinate Al sites, which render AlV sites with strong adsorption capability that facilitates the nucleation of h-CoO NPs. Also, the AlV sites induce the electron transfer from h-CoO to the kaolinite support that results in the upshift of the Co 3d band center and hence improve the H2O2 activation kinetics. Our results demonstrate the superiority of nanoclay as functional supports and could offer a more benign strategy to the solution-phase epitaxy production of functional nanomaterials for diverse applications.

研究领域: 材料科学 · 电化学 · 纳米技术
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ChemistrySelect · 2024 ·Vol. 9 ·期 35 ·e202402622 · IF 1.9

Anchoring Bimetal Zinc–Aluminum Sites on Nitrogen-Doped Carbon Catalyst for Efficient Conversion of CO2 Into Cyclic Carbonates

Wanchang Li,Shuo Wang,Yifei Huang,Limao Fan,Lei Zhang,Kai Huang

Graphical By ingeniously integrating Zn–Al layered double hydroxide with polyaniline, a series of nitrogen-doped carbon catalysts with excellent performance were prepared via in situ polymerization. Diverse cyclic carbonates were synthesized from the corresponding epoxides via the insertion of CO 2 into the β-C─O bond. The design and synthesis of efficient carbon-based materials incorporating multifunctional sites is prospective technology for converting carbon dioxide (CO 2 ) into high-value chemicals. Here, nitrogen-doped carbon catalysts (ZnAl-NC) with bimetal zinc–aluminum sites were synthesized using nitrogen-rich polyaniline (PANI) and ZnAl-LDH through hydrothermal and in situ pyrolysis methods. ZnAl-NC-400, in the presence of tetrabutylammonium bromide (TBAB), exhibited excellent catalytic activity without solvent, achieving high yields (97.2% or 98.5%) in the cycloaddition of CO 2 with propylene oxide (PO) under traditional or mild conditions. NH 3 -TPD and CO 2 -TPD results indicated that the enhanced catalytic activity resulted from the acid–base synergistic effect, involving Lewis acid sites from Zn and Al species and abundant Lewis base sites from the PANI matrix. The impact of calcination temperature on catalyst morphology, structure, and performance was investigated, along with catalyst recycling and adaptability to various epoxides. This work presents an efficient catalyst for CO 2 conversion and suggests new approaches for designing catalytic sites in carbon-based catalysts for CO 2 capture and utilization.

研究领域: 催化化学 · 材料科学 · 环境科学
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INORGANIC CHEMISTRY COMMUNICATIONS · 2025 · IF 5.4

Spatial discriminated aluminum sites in high-silica ERI zeolite for selective O2/N2 separation

Haodong Xie,Yuan Xue,Lei Zhang,Li Liu,Xiang Ni,Wenwen Song,Jingyun Qian,Lei Wang,Hongjun Zhu

The small pore aluminosilicate zeolites are always accompanied by the abundant framework aluminum content and the consequential extra-framework counterparts severely restrained its application in the gas separation process. In this work, the high-silica zeolite ERI (Si/Al = 7.3) was successfully fabricated using a OSDA in the potassium cation medium. It is found that the spatial distribution of aluminum sites in the ERI zeolite can be effectively tailored in the synthetic system with varying aluminum content. Furthermore, the ERI frameworks with spatially biased aluminum sites were also clarified. By combining multiple spectroscopy techniques and powder X-ray diffraction crystallography, the framework of aluminum sites related to host-guest interactions confined in high-silica ERI was clarified. In the gas separation of a binary mixture of O 2 /N 2 (21:79  v /v), the Sr 2+ cation-exchanged high-silica zeolite ERI exhibited efficient O 2 adsorption capacity: 0.74 mmol·g −1 and IAST selectivity: 2.89. These findings not only provide a structural foundation but also offer a model for the efficient separation of O 2 from multi-component gas mixtures.

CAS / MDL: 11138-49-1
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Small · 2023 ·Vol. 20 ·期 17 ·2308632 · IF 13.3

Stable Aluminum Metal Anode Enabled by Dual-Functional Molybdenum Nanoparticles

Shunlong Ju,Qing Qiao,Tian Xu,Zhongchen Zhao,Tengfei Zhang,Guanglin Xia,Xuebin Yu

Constructing robust anode with strong aluminophilicity and rapid desolvation kinetics is essential for achieving high utilization, long-term durability, and superior rate performance in Al metal-based energy storage, yet remains largely unexplored. Herein, molybdenum nanoparticles embedded onto nitrogen-doped graphene (Mo@NG) are designed and prepared as Al host to regulate the deposition behavior and achieve homogeneous Al plating/stripping. The monodispersed Mo nanoparticles reduce the desolvation energy barrier and promote the deposition kinetics of Al. Additionally, Mo nanoparticles act as aluminophilic nucleation sites to minimize the Al nucleation overpotential, further guiding uniform and dense Al deposition. As a result, the dual-functional Mo@NG endows Al anodes with low voltage hysteresis, reversible Al plating/stripping with high coulombic efficiency, and excellent high-rate capability under 5 mA cm −2 . Moreover, the as-designed Al metal full batteries deliver a high capacity retention of 92.8% after 3000 cycles at 1 A g −1 . This work provides an effective solution to optimize the electrochemical properties of Al metal anode from the perspective of desolvation and deposition reactions, towards the development of high-safety and long-cycling aluminum-ion batteries.

研究领域: 材料科学 · 电化学 · 能源存储 · 纳米技术 · 金属负极 · 电池化学 · 界面工程
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