Article
Chemistry, Physical
Congru Gao, Jianwei Li, Jie Zhang, Xiuliang Sun
Summary: A designed binuclear Cu-ZSM-5 catalyst can effectively decompose nitrogen oxides in industrial flue gas and purify the air environment. The catalytic decomposition mechanisms of N2O, NOX-NH3-SCR, and NOX-assisted N2O decomposition over the Cu-ZSM-5 model were simulated using density functional theory method.
Article
Chemistry, Physical
Cui Ouyang, Jianwei Li, Yaqi Qu, Song Hong, Songbo He
Summary: The catalytic oxidation of benzene with N2O to phenol using a hierarchical and microporous Fe/ZSM-5-based catalyst was studied in a continuous fixed bed reactor. In-situ regeneration of the spent catalyst was achieved through oxidative treatment with N2O, and a total of 10 reaction-regeneration cycles were performed. The fresh hierarchical Fe/ZSM-5-Hi2.8 catalyst exhibited excellent performance with 100% N2O conversion, 93.3% phenol selectivity, and a high initial phenol formation rate. However, coke deposition on the catalyst surface led to reversible and irreversible deactivation, reducing the phenol productivity over time.
GREEN ENERGY & ENVIRONMENT
(2023)
Article
Chemistry, Multidisciplinary
Max L. Bols, Julien Devos, Hannah M. Rhoda, Dieter Plessers, Edward Solomon, Robert A. Schoonheydt, Bert F. Sels, Michiel Dusselier
Summary: This study presents a method for preparing highly active alpha-Fe(II) sites by introducing Fe(III) during hydrothermal synthesis and treating appropriately. The effect of iron on zeolite crystallization was investigated, and intermediate iron species were tracked using various spectroscopy techniques.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Energy & Fuels
Jing Li, Suxia Ma, Rongji Cui, Nuo Xu, Ting Pei
Summary: This study prepared fly ash-derived ZSM-5 molecular sieves using an alkali fusion method combined with a hydrothermal method, and analyzed the characteristics of the catalysts synthesized by fly ash and their relationship with catalytic activity through multiple characterization approaches. The results provided important insights into the active sites of catalytic oxidation, indicating that 10% Fe/ZSM-5 catalyst had the best catalytic activity with 92% NO removal efficiency.
Article
Chemistry, Physical
Sara Aranifard, Alexis T. Bell, Frerich J. Keil, Andreas Heyden
Summary: This study investigated the comprehensive reaction mechanism of N2O decomposition over Fe-ZSM-5 catalysts at different temperatures. It was found that different iron species at different temperatures play a crucial role in the catalytic process. The concentration of nitric oxide and water vapor determines the switch between the most dominant active sites.
CATALYSIS SCIENCE & TECHNOLOGY
(2021)
Article
Chemistry, Physical
Michele De Rosa, Simone Morpurgo
Summary: By using DFT calculations, a new coordination for a pair of Cu+ ions at the M6 ring of ZSM-5 was discovered, which is more stable than previously reported structures. After NO adsorption, the Cu+ ions separate and lose the typical reactivity of a Cu-pair. The destabilization of intermediates and transition states at high temperature leads to a decrease in reaction rate. These findings rule out many possibilities in the search for the actual active site for NO decomposition in ZSM-5.
MOLECULAR CATALYSIS
(2022)
Article
Chemistry, Physical
Stepan Sklenak, Thomas Groizard, Hana Jirglova, Petr Sazama, Jiri Dedecek
Summary: Distant binuclear cationic M(II) centers in transitionmetal-exchanged zeolites demonstrate the activation of dioxygen and subsequent oxidation of methane to methanol at room temperature. The reactivity of the alpha-oxygen species with dihydrogen provides valuable insights into their unique characteristics.
JOURNAL OF PHYSICAL CHEMISTRY C
(2022)
Article
Chemistry, Physical
Yujie Liu, Aleksei Bolshakov, Marita Coza, Victor Drozhzhin, Emiel J. M. Hensen, Nikolay Kosinov
Summary: Dehydroaromatization of methane (MDA) under non-oxidative conditions is a promising reaction for direct valorization of natural gas and biogas. Fe-modified ZSM-5 catalysts prepared by direct hydrothermal synthesis, containing isomorphously substituted Fe-sites, exhibit superior MDA activity compared to impregnated Fe/ZSM-5 catalysts. The higher activity of [Fe,Al]ZSM-5 can be attributed to the transformation of tetrahedral Fe3+ into octahedral Fe2+ active sites during the MDA reaction.
Article
Chemistry, Applied
Bin Kang, Ming Li, Zhaoying Di, Xiaonan Guo, Ying Wei, Jingbo Jia, Runduo Zhang
Summary: Anchoring Co2+ ions at Al pairs of ZSM-5 zeolites can enhance the N2O catalytic dissociation performance. Co-ZSM-5 sample derived from the mixture of AlCl3 and TEOS exhibits the best performance. The coordination of Al pairs and the source of Si can affect the catalytic performance and the location of Al pairs.
Article
Chemistry, Physical
Rui Geng, Yacong Liu, Yanxia Guo, Pengfei Wang, Mei Dong, Sen Wang, Jianguo Wang, Zhangfeng Qin, Weibin Fan
Summary: This study systematically investigated the structure evolution and regeneration behavior of Zn-modified ZSM-5 catalysts in ethylene aromatization. The results showed that the generated coke species on spent catalysts can cover acid sites and block pore channels, leading to the transformation of active ZnOH+ species into inactive ZnO. After regeneration, the catalysts were fully recovered and exhibited higher aromatic selectivity.
Article
Chemistry, Multidisciplinary
Jae Geun Yun, Han Min Lee, Gwang Yeol Baik, Ji Yeop Kim, Sang Ji Lee, Min Kyu Jeon, Sang In Keel, Jung Goo Hong
Summary: The study shows that lower O-2 concentrations in a high-temperature thermal reactor facilitate the conversion of N2O to N-2 or NO, while increasing O-2 concentration hinders the conversion process. By introducing a modified parameter, the experimental results align closely with the calculated results.
Article
Chemistry, Applied
Filippo Buttignol, Alberto Garbujo, Pierdomenico Biasi, Daniel Rentsch, Oliver Kroecher, Davide Ferri
Summary: This study investigates the effect of an alumina-based binder on the structure of a commercial Fe-ZSM-5 catalyst. The results show that the binder improves the catalyst's dispersion of Fe species, framework Al content, and acidity, while reducing Fe agglomeration and framework Al migration.
Article
Chemistry, Physical
Kuyyilthodi M. Farhan, Ahammad N. K. Thabassum, Thufail M. Ismail, P. K. Sajith
Summary: Copper exchanged zeolites are effective catalysts for N2O decomposition, but water vapor inhibits the reaction. This study investigates the mechanism of N2O decomposition over dicopper active sites in Cu-ZSM-5 and the inhibitory effect of water on the reaction steps. The findings contribute to understanding complex reactions involving N2O and the influence of water on heterogeneous catalysis.
CATALYSIS SCIENCE & TECHNOLOGY
(2022)
Article
Chemistry, Inorganic & Nuclear
Hai-Jun Li, Rui Feng, Gao-Xiang Wang, Junnian Wei, Zhenfeng Xi
Summary: By reacting semi-rigid PNP ligand with CoBr2, complex PNPCoBr (1) was obtained. The reduction of 1 with excess amounts of KC8 in THE under a N-2 atmosphere yielded binuclear cobalt dinitrogen anion complex [Co(mu-Cy2P)PCyN2](2)K (2) by cleaving the C-P bond of the PNP ligand. Adding 2,2,2-cryptand into complex 2 effectively prepared ion pair Co complex, [Co(mu-Cy2P)PCyN2](2)K(crypt-222) (3). The structures of 1, 2, and 3 were determined by single-crystal X-ray diffraction analysis, and N-2 is moderately activated in complexes 2 and 3. DFT calculations suggest the presence of a Co-Co bond in 2 and 3. Compounds 1 and 2 exhibit catalytic activity for the transformation of N-2 to N(SiMe3)(3).
DALTON TRANSACTIONS
(2022)
Article
Chemistry, Physical
Fan Lin, Tahrizi Andana, Yiqing Wu, Janos Szanyi, Yong Wang, Feng Gao
Summary: N2O decomposition on Cu, Co, and Fe-exchanged SSZ-13 zeolite catalysts follows a dual-site mechanism or a single-site mechanism. The reaction is limited by N-O cleavage under low pressure and first-order kinetic regime. Fe-SSZ-13 exhibits lower activation barriers, leading to a higher N2O decomposition rate.
JOURNAL OF CATALYSIS
(2021)
Article
Chemistry, Physical
Bolun Yu, Denan Li, Qianqian Zhu, Shufan Yao, Lifeng Zhang, Yanshuo Li, Zhenxin Zhang
Summary: This study successfully improved the catalytic activity of a zeolitic octahedral metal oxide by incorporating a single zinc species into its micropore. The zinc incorporation achieved a high ethane conversion rate and ethylene selectivity. Mechanism study showed that the isolated zinc site played a crucial role in activating oxygen and ethane, as well as stabilizing intermediates and transition states.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Ruoqi Liu, Hao Fei, Jian Wang, Ting Guo, Fangyang Liu, Zhuangzhi Wu, Dezhi Wang
Summary: This work successfully synthesized a high-performing S-enriched MoS2 catalyst for electrocatalytic nitrogen reduction reaction (NRR), demonstrating high activity and selectivity. The synergistic effect of the 1T phase and bridging S22- species was shown to play a positive role in NRR performances, and DFT calculations revealed the mechanism behind the improved performance.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Pan Xia, Lele Zhao, Xi Chen, Zhihong Ye, Zhihong Zheng, Qiang He, Ignasi Sires
Summary: This study presents a modified gas-diffusion electrode (GDE) for highly efficient and stable H2O2 electrosynthesis by using trace polymethylhydrosiloxane (PMHS). DFT calculations provide an in-depth understanding of the roles of PMHS functional groups.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Kwangchol Ri, Songsik Pak, Dunyu Sun, Qiang Zhong, Shaogui Yang, Songil Sin, Leliang Wu, Yue Sun, Hui Cao, Chunxiao Han, Chenmin Xu, Yazi Liu, Huan He, Shiyin Li, Cheng Sun
Summary: Different B-doped rGO catalysts were synthesized and their 2e- oxygen reduction reaction (ORR) performance was investigated. It was found that the 2e- ORR selectivity of B-doped rGO was influenced by the B content and oxygen mass transfer conditions. The synthesized catalyst exhibited high 2e- ORR selectivity and was capable of degrading organic pollutants continuously.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Li Lv, Lin Lei, Qi-Wen Chen, Cheng-Li Yin, Huiqing Fan, Jian-Ping Zhou
Summary: Monoclinic phase La2Ti2O7 and orthorhombic phase Bi4Ti3O12 are widely used in photocatalysis due to their layered crystal structure. The electronic structures of these phases play a crucial role in their photocatalytic activity. Heat treatment in a nitrogen atmosphere introduces more oxygen vacancies into the S-scheme heterojunction, leading to enhanced NO removal efficiency.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Choe Earn Choong, Minhee Kim, Jun Sup Lim, Young June Hong, Geon Joon Lee, Keun Hwa Chae, In Wook Nah, Yeomin Yoon, Eun Ha Choi, Min Jang
Summary: In this study, the synergistic effect between argon-plasma-system (AP) and catalysts in promoting the production of reactive species for water remediation was investigated. By altering the oxygen vacancies concentration of CeO2/Bi2O3 catalyst, the production of hydrated electrons was stimulated for PFOA removal. The results showed that the built-in electric field in the Bi/Ce0.43 interface enhanced electron migration and eaq- generation, leading to improved PFOA removal efficiency.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Yushan Wu, Di Xu, Yanfei Xu, Xin Tian, Mingyue Ding
Summary: Efficient synthesis of primary amines from carbonyl compounds was achieved via reductive amination using Ru@NC-Al2O3 as a catalyst, exhibiting high activity and selectivity under mild conditions.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Yilan Jiang, Peifang Wang, Tingyue Chen, Keyi Gao, Yiran Xiong, Yin Lu, Dionysios D. Dionysiou, Dawei Wang
Summary: By controlling the content of Co and Ni in Co1-xNixFe2O4, the production of O-1(2) from H2O2 can be regulated. NiFe2O4, with the lowest lattice distortion degree, can efficiently produce O-1(2) as the dominant reactive oxygen species. The system also exhibits significant resistance to water matrix interference.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Shuai Feng, Donglian Li, Hao Dong, Song Xie, Yaping Miao, Xuming Zhang, Biao Gao, Paul K. Chu, Xiang Peng
Summary: In this study, MoO2/Mo2N heterostructures were prepared by regulating the coordination of Mo atoms. The electrocatalyst exhibits high current density and excellent stability for hydrogen evolution reaction.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Jia-Cheng E. Yang, Min -Ping Zhu, Daqin Guan, Baoling Yuan, Darren Delai Sun, Chenghua Sun, Ming-Lai Fu
Summary: This study successfully modulated the electron configuration and spin state of millimetric metal catalysts by adjusting the support curvature radius. The electronic structure-oriented spin catalysis was found to affect the degradation of pollutants, providing new insights for the design and production of highly active, reusable, and stable catalysts.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Tao Zhong, Su Tang, Wenbin Huang, Wei Liu, Huinan Zhao, Lingling Hu, Shuanghong Tian, Chun He
Summary: In this study, a highly efficient photocatalyst for the elimination of CH3SH was developed by engineering different crystal facets and coupling them with PHI. Cu (111)/PHI exhibited the highest elimination efficiency and showed good stability and reusability. The enhanced surface electron pump effect and effective adsorption mechanisms were revealed through comprehensive characterizations and DFT calculations.
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY
(2024)
Article
Chemistry, Physical
Feifei Yang, Tianyu Zhang, Jiankang Zhao, Wei Zhou, Nicole J. Libretto, Jeffrey T. Miller
Summary: A Ni3Sn intermetallic nano particle was found to have geometrically isolated Ni sites that could selectively cleave C-O bonds in biomass derivatives. This nano particle showed high activity and selectivity towards 2-methylfuran, unlike Ni nanoparticles that produced other unwanted products derived from the aromatic rings.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Chemistry, Physical
Lulu Qiao, Di Liu, Anquan Zhu, Jinxian Feng, Pengfei Zhou, Chunfa Liu, Kar Wei Ng, Hui Pan
Summary: This study reveals that surface evolution plays a crucial role in enhancing the electrocatalytic performance of transition metal oxides for electrochemical nitrate reduction reaction (e-NO3RR). Incorporating nickel into Co3O4 can promote surface reconstruction and improve the adsorption of intermediates and reduce energy barriers, leading to enhanced catalytic performance. The reconstructed cobalt-nickel hydroxides (CoyNi1_y(OH)2) on the catalyst's surface serve as the active phase.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Chemistry, Physical
Xinyu Song, Yang Shi, Zelin Wu, Bingkun Huang, Xinhao Wang, Heng Zhang, Peng Zhou, Wen Liu, Zhicheng Pan, Zhaokun Xiong, Bo Lai
Summary: This study explores the discriminative activities and mechanisms for activation of O-O bond in peroxy compounds via single-atom catalysts (SACs) with higher coordination numbers (M-N5). The atomic catalyst (Fe-SAC) with Fe-N5 as the active center was constructed, effectively activating peroxymonosulfate (PMS), peroxydisulfate (PDS), and hydrogen peroxide (H2O2). The study demonstrates the degradation efficiencies of acyclovir are related to the O-O bond length in different peroxy compounds, and reveals the discriminative mechanisms for activation of O-O bond in different Fenton-like systems.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)
Article
Chemistry, Physical
Yangzhuo He, Hong Qin, Ziwei Wang, Han Wang, Yuan Zhu, Chengyun Zhou, Ying Zeng, Yicheng Li, Piao Xu, Guangming Zeng
Summary: A dual-metal-organic framework (MOF) assisted strategy was proposed to construct a magnetic Fe-Mn oxycarbide anchored on N-doped carbon for peroxymonosulfate (PMS) activation. The FeMn@NC-800 catalyst exhibited superior activity with almost 100% degradation of sulfamethazine (SMZ) in 30 minutes. The study provided insights for the rational design of high-performance heterogeneous catalysts and proposed a novel nonradical-based catalytic oxidation for environmental cleaning.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2024)