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Results in Journal ACS Catalysis: 9,014

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Ken Yamazaki, Pablo Gabriel, Graziano Di Carmine, Julia Pedroni, Mirxan Farizyan, ,
ACS Catalysis pp 7489-7497; doi:10.1021/acscatal.1c01589

Abstract:
An iridium-catalyzed reductive generation of both stabilized and unstabilized azomethine ylides and their application to functionalized pyrrolidine synthesis via [3 + 2] dipolar cycloaddition reactions is described. Proceeding under mild reaction conditions from both amide and lactam precursors possessing a suitably positioned electron-withdrawing or a trimethylsilyl group, using 1 mol% Vaska’s complex [IrCl(CO)(PPh3)2] and tetramethyldisiloxane (TMDS) as a terminal reductant, a broad range of (un)stabilized azomethine ylides were accessible. Subsequent regio- and diastereoselective, inter- and intramolecular dipolar cycloaddition reactions with variously substituted electron-deficient alkenes enabled ready and efficient access to structurally complex pyrrolidine architectures. Density functional theory (DFT) calculations of the dipolar cycloaddition reactions uncovered an intimate balance between asynchronicity and interaction energies of transition structures, which ultimately control the unusual selectivities observed in certain cases.
Qi Liu, Xinyue Xie, Mancheng Tang, Wentao Tao, , Yuanzhen Zhang, Tingting Huang, , Zixin Deng,
ACS Catalysis pp 7477-7488; doi:10.1021/acscatal.1c01229

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María Galiana-Cameo, Asier Urriolabeitia, Eduardo Barrenas, , , , , Ricardo Castarlenas
ACS Catalysis pp 7553-7567; doi:10.1021/acscatal.1c00602

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Feilong Sun, Ting Wang, Gui-Juan Cheng, Xianjie Fang
ACS Catalysis pp 7578-7583; doi:10.1021/acscatal.1c01971

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Jeonghoon Lim, Chun-Yen Liu, Jinho Park, Yu-Hsuan Liu, , ,
ACS Catalysis pp 7568-7577; doi:10.1021/acscatal.1c01413

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Jia Du, , Alessandro Zana,
ACS Catalysis pp 7584-7594; doi:10.1021/acscatal.1c01496

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Shao-Qing Liu, Min-Rui Gao, , Lu Gong, ,
ACS Catalysis pp 7604-7612; doi:10.1021/acscatal.1c01899

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Yiliguma, Sang-Won Park, Jiang Li, Masato Sasase, ,
ACS Catalysis pp 7595-7603; doi:10.1021/acscatal.1c01646

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Siuli Das, Rakesh Mondal, Gargi Chakraborty, Amit Kumar Guin, Abhishek Das,
ACS Catalysis pp 7498-7512; doi:10.1021/acscatal.1c00275

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Jie Wang, Xue Dong, Jing Liu, Wenzhen Li, , ,
ACS Catalysis pp 7422-7428; doi:10.1021/acscatal.1c01284

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Mengru Li, ,
ACS Catalysis pp 7411-7421; doi:10.1021/acscatal.1c01406

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Xingwang Lan, Xiaopeng Liu, Yize Zhang, Qing Li, Juan Wang, Qianfan Zhang,
ACS Catalysis pp 7429-7441; doi:10.1021/acscatal.1c01794

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Yi Cheng Kang, Sean M. Treacy,
ACS Catalysis pp 7442-7449; doi:10.1021/acscatal.1c02285

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Hiroaki Fujita, ,
ACS Catalysis pp 7460-7466; doi:10.1021/acscatal.1c01344

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Philipp S. Steinlandt, Xiulan Xie, Sergei Ivlev,
ACS Catalysis pp 7467-7476; doi:10.1021/acscatal.1c01675

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Xiaohang Li, Xiaoxuan Yang, Liting Liu, He Zhao, Yawei Li, Haiyan Zhu, Yuanzhen Chen, Shengwu Guo, Yongning Liu, , et al.
ACS Catalysis pp 7450-7459; doi:10.1021/acscatal.0c05446

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Kun Chen, Yang Hu, ,
ACS Catalysis pp 7358-7370; doi:10.1021/acscatal.1c01062

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Liam J. Donnelly, Teresa Faber, Carole A. Morrison, Gary S. Nichol, ,
ACS Catalysis pp 7394-7400; doi:10.1021/acscatal.1c00869

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, Chia-Nung Kuo, , Andrea Marchionni, Gianluca D’Olimpio, Jonathan Filippi, Silvia Mauri, Piero Torelli, Chin Shan Lue, Francesco Vizza, et al.
ACS Catalysis pp 7311-7318; doi:10.1021/acscatal.1c01653

Abstract:
Recently, several researchers have claimed the existence of superior catalytic activity associated with topological materials belonging to the class of Dirac/Weyl semimetals, owing to the high electron conductivity and charge carrier mobility in these topological materials. By means of X-ray photoelectron spectroscopy, electrocatalytic tests, and density functional theory, we have investigated the chemical reactivity (chemisorption of ambient gases), ambient stability, and catalytic properties of PdSn4, a topological semimetal showing Dirac node arcs. We find a Tafel slope of 83 mV in the hydrogen evolution reaction (HER) dec–1 with an overpotential of 50 mV, with performances resembling those of pure Pd, regardless of its limited amount in the alloy, with a subsequent reduction in the cost of raw materials by ∼80%. Remarkably, the PdSn4-based electrode shows superior robustness to CO compared to pure Pd and Pt and high stability in water media, although the PdSn4 surface is prone to oxidation with the formation of a sub-nanometric SnO2 skin. Moreover, we also assessed the significance of the role of topological electronic states in the observed catalytic properties. Actually, the peculiar atomic structure of oxidized PdSn4 enables the migration of hydrogen atoms through the Sn–O layer with a barrier comparable with the energy cost of the Heyrovsky step of HER over Pt(111) in acidic media (0.1 eV). On the other hand, the topological properties play a minor role, if existing, contrarily to the recent reports overestimating their contribution in catalytic properties.
Xuning Li, YaQiong Zeng, Ching-Wei Tung, Ying-Rui Lu, Sambath Baskaran, Sung-Fu Hung, Shifu Wang, , , Ting-Shan Chan, et al.
ACS Catalysis pp 7292-7301; doi:10.1021/acscatal.1c01621

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Teng Li, Arik Beck, , , Manoj K. Ghosalya, Maneka Roger, , , , , et al.
ACS Catalysis pp 7371-7382; doi:10.1021/acscatal.0c04868

Abstract:
Zeolite-supported metal catalysts are widely employed in a number of chemical processes, and the stability of the catalytically active species is one of the most critical factors determining the reaction performance. A good example is the Pd/zeolite catalyst, which provides high activity for methane oxidation but deactivates rapidly under the reaction conditions due to palladium nanoparticle sintering. Although coating the metals with thin shells of porous materials is a promising strategy to address the sintering of metals, it is still challenging to fix small metal particles completely inside zeolite crystals. Here, using an amine-based ligand to stabilize palladium during the zeolite synthesis, we realize the exclusive encapsulation of highly dispersed palladium oxide clusters (1.8–2.8 nm) in the microporous channels and voids of the nanosized silicalite-1 crystals. The synthesis conditions of the zeolite-supported catalyst influence the encapsulation degree and the size distribution of metal particles. Thanks to the encapsulation effect of small palladium oxide clusters, together with the inherent properties of silicalite-1 such as low acidity, high hydrophobicity, and high hydrothermal stability, the optimized [email protected] catalyst outperforms the traditional Pd-based catalysts prepared by wetness impregnation, exhibiting both high activity and better stability in the lean methane oxidation reaction.
Zhuo Chen, Meijie Zhu, Mengwei Cai, Lulu Xu, Yiyi Weng
ACS Catalysis pp 7401-7410; doi:10.1021/acscatal.1c01417

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Xuchao Wang, Feipeng Liu, Zijuan Yan, Qing Qiang, Wei Huang, Zi-Qiang Rong
ACS Catalysis pp 7319-7326; doi:10.1021/acscatal.1c00951

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Anja Knorrscheidt, Jordi Soler, Nicole Hünecke, Pascal Püllmann, ,
ACS Catalysis pp 7327-7338; doi:10.1021/acscatal.1c00847

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Peidong Song, Linlin Hu, Tao Yu, Jiao Jiao, Yangqing He, Liang Xu,
ACS Catalysis pp 7339-7349; doi:10.1021/acscatal.1c01671

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Sayan Kar, Yinjun Xie, Quan Quan Zhou, , Yehoshoa Ben-David,
ACS Catalysis pp 7383-7393; doi:10.1021/acscatal.1c00728

Abstract:
The current existing methods for the amide bond synthesis via acceptorless dehydrogenative coupling of amines and alcohols all require high reaction temperatures for effective catalysis, typically involving reflux in toluene, limiting their potential practical applications. Herein, we report a system for this reaction that proceeds under mild conditions (reflux in diethyl ether, boiling point 34.6 °C) using ruthenium PNNH complexes. The low-temperature activity stems from the ability of Ru–PNNH complexes to activate alcohol and hemiaminals at near-ambient temperatures through the assistance of the terminal N–H proton. Mechanistic studies reveal the presence of an unexpected aldehyde-bound ruthenium species during the reaction, which is also the catalytic resting state. We further utilize the low-temperature activity to synthesize several simple amide bond-containing commercially available pharmaceutical drugs from the corresponding amines and alcohols via the dehydrogenative coupling method.
Hang-Dong Zuo, Shan-Shan Zhu, Wen-Juan Hao, Shi-Chao Wang, ,
ACS Catalysis pp 7310-7310; doi:10.1021/acscatal.1c02278

Tareq A. Al-Attas, Nedal N. Marei, Xue Yong, Nael G. Yasri, , , ,
ACS Catalysis pp 7350-7357; doi:10.1021/acscatal.1c01506

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Hiroshi Yoshida, Haruka Oyama, Ryo Shiomori, Taiki Hirakawa, , Masato Machida
ACS Catalysis pp 7302-7309; doi:10.1021/acscatal.1c01419

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Haoyu Tang, Yijie Tang, Igor V. Kurnikov, Hsuan-Jen Liao, , , ,
ACS Catalysis pp 7186-7192; doi:10.1021/acscatal.1c01150

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ACS Catalysis, Volume 11; doi:10.1021/csv011i011_1484671

ACS Catalysis, Volume 11, pp 7257-7269; doi:10.1021/acscatal.1c00688

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Weixiang Shang, Mingyang Gao, Yuchao Chai, Guangjun Wu, Naijia Guan,
ACS Catalysis, Volume 11, pp 7249-7256; doi:10.1021/acscatal.1c00950

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Zhengyu Han, Gang Liu, Xuanliang Yang, , Xumu Zhang
ACS Catalysis, Volume 11, pp 7281-7291; doi:10.1021/acscatal.1c01353

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Michael J. Cordon, Junyan Zhang, Stephen C. Purdy, Evan C. Wegener, Kinga A. Unocic, Lawrence F. Allard, Mingxia Zhou, Rajeev S. Assary, , Theodore R. Krause, et al.
ACS Catalysis, Volume 11, pp 7193-7209; doi:10.1021/acscatal.1c01136

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Geyla C. Dubed Bandomo, Suvendu Sekhar Mondal, Federico Franco, Alberto Bucci, , , Phebe H. van Langevelde, , ,
ACS Catalysis, Volume 11, pp 7210-7222; doi:10.1021/acscatal.1c00314

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ACS Catalysis, Volume 11; doi:10.1021/csv011i011_1484670

, Yu-Cheng Su, Chia-Hao Lu, Chien-I Lien, Shiang-Fu Hung, Chan-Wei Hsu, Rachit Agarwal, Ramuasagar Modala, Hung-Min Tseng, Pin-Xuan Tseng, et al.
ACS Catalysis, Volume 11, pp 7160-7175; doi:10.1021/acscatal.1c01813

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Xiangjuan Qi, Ronglin Zhong, Mengmeng Chen, Chunyi Sun, Siqi You, Jianxia Gu, , Dongxu Cui, ,
ACS Catalysis, Volume 11, pp 7241-7248; doi:10.1021/acscatal.1c01974

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Basujit Chatterjee, Soumyashree Jena, Vishal Chugh, ,
ACS Catalysis, Volume 11, pp 7176-7185; doi:10.1021/acscatal.1c00733

Abstract:
The direct synthesis of amides and nitriles from readily available aldehyde precursors provides access to functional groups of major synthetic utility. To date, most reliable catalytic methods have typically been optimized to supply one product exclusively. Herein, we describe an approach centered on an operationally simple iron-based system that, depending on the reaction conditions, selectively addresses either the C═O or C–H bond of aldehydes. This way, two divergent reaction pathways can be opened to furnish both products in high yields and selectivities under mild reaction conditions. The catalyst system takes advantage of iron’s dual reactivity capable of acting as (1) a Lewis acid and (2) a nitrene transfer platform to govern the aldehyde building block. The present transformation offers a rare control over the selectivity on the basis of the iron system’s ionic nature. This approach expands the repertoire of protocols for amide and nitrile synthesis and shows that fine adjustments of the catalyst system’s molecular environment can supply control over bond activation processes, thus providing easy access to various products from primary building blocks.
Ana M. Geer, Charles Musgrave Iii, Christopher Webber, , Bradley A. McKeown, Chang Liu, , Peter Jakes, Xiaofan Jia, , et al.
ACS Catalysis, Volume 11, pp 7223-7240; doi:10.1021/acscatal.1c01395

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Shaoguang Zhang, Serge Ruccolo, , Artis Klapars, Nicholas Marshall,
ACS Catalysis, Volume 11, pp 7270-7280; doi:10.1021/acscatal.1c01037

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Beom-Sik Kim, Junemin Bae, Hojin Jeong, ChanYeong Choe,
ACS Catalysis, Volume 11, pp 7154-7159; doi:10.1021/acscatal.1c02209

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, Nozomi Ohara, Shrikant M. Khake,
ACS Catalysis, Volume 11, pp 7126-7131; doi:10.1021/acscatal.1c01901

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Chao-Peng Wang, Yang Feng, Hao Sun, Yurou Wang, Jun Yin, , ,
ACS Catalysis, Volume 11, pp 7132-7143; doi:10.1021/acscatal.1c01447

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Masanori Inaba, Alessandro Zana, , Francesco Bizzotto, Carsten Dosche, Alexandra Dworzak, , , Luise Theil Kuhn,
ACS Catalysis, Volume 11, pp 7144-7153; doi:10.1021/acscatal.1c00652

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Emily J. Mazeau, Priyanka Satpute, Katrín Blöndal, ,
ACS Catalysis, Volume 11, pp 7114-7125; doi:10.1021/acscatal.0c04100

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Fang-Fang Feng, Xuan-Yu Liu, Chi Wai Cheung, Jun-An Ma
ACS Catalysis, Volume 11, pp 7070-7079; doi:10.1021/acscatal.1c01840

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