Article
Chemistry, Physical
Guo Chen, Piao He, Chao Liu, Xiu-Fang Mo, Jing-Jing Wei, Ze-Wen Chen, Tao Cheng, Li-Zhi Fu, Xiao-Yi Yi
Summary: Due to its high energy requirement and favourable subsequent conversion, the synthesis of hydrazine remains a challenge. This study demonstrates that ruthenium complexes bearing 2-[5-(pyridin-2-yl)-1H-pyrrol-2-yl]pyridine ligands exhibit high catalytic activity for the direct electrochemical oxidation of ammonia to generate hydrazine in acetonitrile.
Article
Chemistry, Multidisciplinary
Chaeeun Lim, Hyogyun Roh, Eun Ho Kim, Hangyeol Kim, Taiho Park, Donghwa Lee, Kijung Yong
Summary: In order to achieve global carbon neutrality, research has focused on developing green ammonia production methods to replace the Haber-Bosch process. The nitrate reduction reaction (NO3RR) has gained attention for electrochemically producing ammonia from nitrate and purifying wastewater simultaneously. This study demonstrates the use of tungsten phosphide (WP) nanowires as cathode electrocatalysts for NO3RR, which have high efficiency and activity in both neutral and alkaline media.
Article
Nanoscience & Nanotechnology
Wentao Wang, Qizhu Qian, Yapeng Li, Yin Zhu, Yafei Feng, Mingyu Cheng, Huaikun Zhang, Yangyang Zhang, Genqiang Zhang
Summary: Hydrazine oxidation-assisted water electrolysis is a promising method for energy-efficient electrochemical hydrogen production and decomposition of hydrazine-rich wastewater. However, developing highly active catalysts remains challenging. In this study, we demonstrate the use of Ru nanoparticles supported on hollow N-doped carbon microtubes as bifunctional electrocatalysts for HER and HzOR. The hierarchical Ru NPs/H-NCMTs exhibit excellent electrocatalytic activity in alkaline conditions, with low overpotential for HER and HzOR. The assembled hybrid electrolyzer using Ru NPs/H-NCMT catalysts shows low cell voltage and remarkable stability. Density functional theory calculations reveal that Ru NPs serve as active sites for both HER and HzOR, enhancing their performances. This work provides a novel avenue for efficient and stable electrocatalysts for hydrogen production.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Shi He, Yufeng Chen, Mengdi Wang, Hanggai Nuomin, Peter Novello, Xueqian Li, Siyuan Zhu, Jie Liu
Summary: Ammonia is a promising hydrogen mediator that reduces the cost of hydrogen transportation, but improvements are needed for extracting hydrogen. Ammonia electrolysis is a convenient method for low-cost hydrogen production. Nickel-cobalt nitride nanosheets show high electrocatalytic activity for the ammonia oxidation reaction in non-aqueous solutions.
Article
Chemistry, Physical
Huimin Zhang, Hailong Wang, Luanqi Zhou, Qiming Li, Xu Yang, Yifei Wang, Meng Zhang, Zucheng Wu
Summary: Direct electrochemical oxidation of ammonia-nitrogen wastewater is a challenging task. This study synthesized NiCu3-N-C diatomic site catalyst (DAC) via solid-phase pyrolysis and demonstrated its high dispersion and micro-environment characteristics. The results showed that NiCu3-N-C DAC exhibited excellent intrinsic activity and achieved high removal efficiency, faradaic efficiency, and N-2 selectivity in a real wastewater experiment. This work provides a good example of designing functionally coordinated DACs for efficient ammonia-nitrogen wastewater treatment.
APPLIED CATALYSIS B-ENVIRONMENTAL
(2023)
Article
Multidisciplinary Sciences
Takayuki Itabashi, Kazuya Arashiba, Akihito Egi, Hiromasa Tanaka, Keita Sugiyama, Shun Suginome, Shogo Kuriyama, Kazunari Yoshizawa, Yoshiaki Nishibayashi
Summary: Dinitrogen is a valuable material for the synthesis of organonitrogen compounds. This study presents a catalytic reaction for the formation of cyanate anion from dinitrogen under ambient conditions. The use of molybdenum-PNP complexes as catalysts enables the synthesis of NCO- from dinitrogen in two steps.
NATURE COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Qizhu Qian, Wentao Wang, Gongrui Wang, Xiaoyue He, Yafei Feng, Ziyun Li, Yin Zhu, Yangyang Zhang, Genqiang Zhang
Summary: This study presents an energy-saving approach to produce high-purity hydrogen through hydrazine-assisted hybrid water electrolysis. By synthesizing the RuP/C-PAN catalyst, the water electrolysis reaction can be driven at ultralow voltage under different pH values, and the catalytic mechanism is explained. This research contributes to transcending the limitation on the pH value of electrolytes and advancing the development of an energy-saving hydrogen generation technique based on emerging hybrid water electrolysis.
Article
Chemistry, Multidisciplinary
Hiroki Toda, Kaito Kurok, Ryoichi Kanega, Tasuku Yano, Takeshi Yoshikawa, Shogo Kuriyama, Yuichiro Himeda, Ken Sakata, Yoshiaki Nishibayashi
Summary: We investigated the catalytic ammonia oxidation using ruthenium complexes as catalysts under electrochemical conditions and found that the ruthenium complex bearing phthalazines showed the highest catalytic activity.
BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN
(2023)
Article
Chemistry, Physical
Jitendra Shashikant Samdani, Jakkid Sanetuntikul, Sangaraju Shanmugam
Summary: The electrochemical oxidation of urea and hydrazine over self-supported Fe-doped Ni3S2/NF nanostructured material is investigated. The Fe-Ni3S2/NF-2 prepared at specific conditions shows promising results in the oxidation reactions of hydrazine and urea. The improvement in the chemical kinetics of urea and hydrazine oxidation is attributed to the synergistic effect of adsorption and fast electron transfer on Fe-Ni3S2/NF-2. This study has implications for hydrogen energy applications.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Chemistry, Multidisciplinary
Zengxiang Lv, Leiduan Hao, Zhibo Yao, Weixiang Li, Alex W. Robertson, Zhenyu Sun
Summary: This research discovered that anolytes containing halide ions have a profound impact on the electrochemical synthesis of ammonia, intensifying the crossover of ammonium. Additionally, external factors such as applied potentials and Cl- concentration are closely associated with the migration and oxidation of ammonium.
Article
Chemistry, Physical
Shi He, Vasishta Somayaji, Mengdi Wang, Seung-Hoon Lee, Zhijia Geng, Siyuan Zhu, Peter Novello, Chakrapani V. Varanasi, Jie Liu
Summary: The study demonstrates that high entropy oxides have great electrocatalytic activity for ammonia oxidation, indicating a potential pathway for energy release. XPS analysis suggests that the balancing metal d-band of Mn and Cu cations contributes to long-lasting electrocatalytic activity.
Article
Chemistry, Organic
Aline A. N. de Souza, Aloisio de A. Bartolomeu, Timothy J. Brocksom, Timothy Noel, Kleber T. de Oliveira
Summary: The electrochemical sulfenylation reaction was investigated in both batch and continuous flow regimes, with quaternary ammonium salts identified as the best mediators. The tolerance of Boc-cysteine to the reaction protocol was noted, increasing its relevance. The methodology was found to be scalable in both batch and continuous flow conditions, offering potential for further studies involving important functional groups in organic synthesis.
JOURNAL OF ORGANIC CHEMISTRY
(2022)
Article
Multidisciplinary Sciences
Xiaorong Zhu, Xiaocheng Zhou, Yu Jing, Yafei Li
Summary: The study systematically investigates the catalytic activity of three experimental two-dimensional metal borides (MBenes) for urea synthesis, demonstrating the potential of Mo2B2 and Cr2B2 as effective electrocatalysts for urea production.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Multidisciplinary
Nina X. Gu, Paul H. Oyala, Jonas C. Peters
Summary: The formation of Ni-III-NH2 species that undergo bimolecular coupling to generate a Ni-2(II)(N2H4) complex is discussed in this study. Further oxidation to a structurally unusual Ni-2(N2H2) species releases N-2, establishing a synthetic cycle for Ni-mediated AO using Earth-abundant, late first-row metals.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Physical
Tejs Vegge, Ping Chen
Summary: A new class of catalysts based on ternary ruthenium complex hydrides has been developed for low-temperature ammonia synthesis. These catalysts support a non-dissociative reaction path for dinitrogen reduction, with lithium or barium cations stabilizing the intermediates and [RuH6](4-) anionic centers facilitating an energetically balanced multi-step reaction for ammonia synthesis.
Article
Chemistry, Multidisciplinary
Shang-Qian Li, Lin-Fang Dai, Yi-Qi Tian, Yi-Xiao Yi, Jun Yan, Chao Liu
Summary: In this study, a large polymolybdate-templated {Ag49Mo16} cluster protected by six thiacalix[4]arene (TC4A) molecules was synthesized. Structural analysis revealed that the {Ag49Mo16} cluster is assembled by inserting a [Mo6O22](8-) cluster into a [Ag49Mo10@(TC4A)(6)] cage. The solution stability and photoelectric properties of {Ag49Mo16} were discussed, and its electrocatalytic CO2 reduction application showed promising results with a CO faradaic efficiency (FE) of 44.75% at -0.8 V (vs. RHE).
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Inorganic & Nuclear
Lin-Fang Dai, Xue-Ru Liu, Yi-Qi Tian, Xiao-Yi Yi, Chao Liu
Summary: This study synthesized six TBC[6]-stabilized titanium-oxo clusters (TOCs) using TBC[6] as the ligand. The introduction of auxiliary carboxylic ligands led to the growth of cluster structures, increasing the variety of TOCs. The clusters showed potential as recyclable heterogeneous photocatalysts for the oxidation of sulfide to sulfoxide.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Yue Liu, Pingping Yi, Lishan Gong, Xiaoyi Yi, Piao He, Tingwei Wang, Jianguo Zhang
Summary: Heat-resistant explosives are crucial in specialized applications. Two new energetic metal-organic frameworks (EMOFs), potassium 4,4'-oxybis[3,3'-(5-tetrazol)]furazan and potassium (1,2,4-triazol-3-yl)tetrazole, with a three-dimensional structure, were synthesized and characterized. The EMOFs exhibited high thermostability, positive heat of formation, and suitable sensitivities, making them promising heat resistant explosives.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Xiu-Fang Mo, Shun Ge, Ping-Ping Yi, Guo Chen, Jia-Hao Liu, Chao Liu, Xiao-Yi Yi, Piao He
Summary: A series of Cp*Ir complexes with N^N or N^O ancillary ligands were designed and synthesized, and it was found that the pendant base in metal complexes plays a key role in rate-determining heterolytic H2 splitting and enhancing the proton transfer, thereby improving the catalytic activity.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Shun Ge, Lishan Gong, Pingping Yi, Xiufang Mo, Chao Liu, Xiao-Yi Yi, Piao He
Summary: A series of novel Cp*Ir complexes with nitrogen-rich NN bidentate ligands were developed for efficient catalytic dehydrogenation of formic acid in water. The study reveals the influence of ligand structure and water-assisted reaction steps on the catalytic activity, and proposes a plausible reaction mechanism.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Liang-Jun Li, Yu-Ting Luo, Yi-Qi Tian, Pu Wang, Xiao-Yi Yi, Jun Yan, Yong Pei, Chao Liu
Summary: In this study, a thiacalix[4]arene-protected Ag-30 nanocluster with high stability and catalytic activity was presented. The Ag-30 nanocluster features a metallic core shielded by {Ag-5@(TC4A)(4)} motifs. It was found that the catalytic activity of Ag-30 is higher than that of Ag-1(8)n, possibly due to the greater stability of the dual adsorption mode of the *COOH intermediate on the metallic core.
INORGANIC CHEMISTRY
(2023)
Article
Chemistry, Inorganic & Nuclear
Meng Xue, Dan-Ling Zhuang, Li-Zhi Fu, Guo Chen, Jiaying Su, Jun Zhu, Xiao-Yi Yi
Summary: The visible-light-mediated dearomatisation of pyrroles is a powerful strategy for synthesizing pharmaceuticals and bioactive compounds. In this study, we report a chemiluminescent reaction between a pyrrole metalated-Ir(III) complex and singlet oxygen, resulting in the formation of a ketoamide complex. The reaction mechanism of this metalated pyrrole-singlet oxygen reaction under irradiation is investigated through experiment and DFT calculations.
Article
Chemistry, Inorganic & Nuclear
Wen-Lei Mu, Linlin Wu, Wei-Dong Yu, Xiao-Yi Yi, Jun Yan, Chao Liu
Summary: Accurate manipulation of ligands in clusters is challenging but important for controlling the properties and catalytic activity. In this study, two Cu(ii)-thiacalix[4]arene metallamacrocycles with different topologies were designed and synthesized, and the ligand substitution was successfully achieved. The effect of ligand tailoring on the electronic structure of clusters was revealed using theoretical calculations. The clusters showed promising catalytic activity for selective sulfide oxidation.
DALTON TRANSACTIONS
(2023)
Article
Chemistry, Multidisciplinary
Yi-Qi Tian, Wen-Lei Mu, Lin-Lin Wu, Xiao-Yi Yi, Jun Yan, Chao Liu
Summary: This study introduces a novel strategy to synthesize a unique Ag/Ti bimetallic nanocluster, which exhibits exceptional catalytic activity in the electroreduction of CO2. The identification of specific Ag sites with high catalytic activity provides valuable insights for the design of efficient CO2 reduction catalysts.
Article
Chemistry, Physical
Guo Chen, Piao He, Chao Liu, Xiu-Fang Mo, Jing-Jing Wei, Ze-Wen Chen, Tao Cheng, Li-Zhi Fu, Xiao-Yi Yi
Summary: Due to its high energy requirement and favourable subsequent conversion, the synthesis of hydrazine remains a challenge. This study demonstrates that ruthenium complexes bearing 2-[5-(pyridin-2-yl)-1H-pyrrol-2-yl]pyridine ligands exhibit high catalytic activity for the direct electrochemical oxidation of ammonia to generate hydrazine in acetonitrile.
Article
Chemistry, Multidisciplinary
Yi-Qi Tian, Wen-Lei Mu, Lin-Lin Wu, Xiao-Yi Yi, Jun Yan, Chao Liu
Summary: In this study, a unique Ag/Ti bimetallic nanocluster (Ti8Ag8) was synthesized as an exceptional CO2 electroreduction catalyst, surpassing the performance of a Ti2Ag4 cluster. The study provides valuable insights into the accurate identification of catalytic sites in bimetallic nanoclusters and opens up promising avenues for efficient CO2 reduction catalyst design.
Article
Chemistry, Multidisciplinary
Yi-Qi Tian, Yun-Shu Cui, Jia-Hui Zhu, Cong-Qiao Xu, Xiao-Yi Yi, Jun Li, Chao Liu
Summary: This paper reports a novel titanium-based coordination cage assembled from titanium nodes and oriented ligands. The cage exhibits tunable properties and demonstrates strong photocatalytic H-2 evolution activity.
CHEMICAL COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Yue Liu, Lishan Gong, Xiaoyi Yi, Piao He, Jianguo Zhang
Summary: A methodology combining linkage groups and substituted fragments with 1,2,3-triazole-N-oxide series was used to design 48 novel high energy density materials. The analysis of the electronic structure and detonation properties showed the correlations between structure and properties in this series.
NEW JOURNAL OF CHEMISTRY
(2022)
Article
Chemistry, Multidisciplinary
Yi-Qi Tian, Yun-Shu Cui, Wei-Dong Yu, Cong-Qiao Xu, Xiao-Yi Yi, Jun Yan, Jun Li, Chao Liu
Summary: In this study, we report a metallocalixarene nanocage cluster based on Ti(Ⅳ) ions, which exhibits remarkable stability and can act as a stable photocatalyst for the oxidation of ammonia to imines in high-concentration acid/alkali solutions.
CHEMICAL COMMUNICATIONS
(2022)