Yuhui Chen, Dr. Rui Zhang, Prof. Hsiao-Tsu Wang, Dr. Ying-Rui Lu, Dr. Yu-Cheng Huang, Dr. Yu-Chun Chuang, Prof. Hua Wang, Prof. Jun Luo, Prof. Lili Han
{"title":"Temperature-Dependent Structures of Single-Atom Catalysts","authors":"Yuhui Chen, Dr. Rui Zhang, Prof. Hsiao-Tsu Wang, Dr. Ying-Rui Lu, Dr. Yu-Cheng Huang, Dr. Yu-Chun Chuang, Prof. Hua Wang, Prof. Jun Luo, Prof. Lili Han","doi":"10.1002/asia.202300679","DOIUrl":"10.1002/asia.202300679","url":null,"abstract":"<p>Single-atom catalysts (SACs) have the unique coordination environment and electronic structure due to the quantum size effect, which plays an essential role in facilitating catalytic reactions. However, due to the limited understanding of the formation mechanism of single atoms, achieving the modulation of the local atomic structure of SACs is still difficult and challenging. Herein, we have prepared a series of Ni SACs loaded on nitrogen-doped carbon substrates with different parameters using a dissolution-and-carbonization method to systematically investigate the effect of temperature on the structure of the SACs. The results of characterization and electrochemical measurements are analyzed to reveal the uniform law between temperature and the metal loading, bond length, coordination number, valence state and CO<sub>2</sub> reduction performance, showing the feasibility of controlling the structure of SACs through temperature to regulate the catalytic performance. This is important for the understanding of catalytic reaction mechanisms and the design of efficient catalysts.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10554829","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dr. Taylor D. Krueger, Dr. Cheng Chen, Prof. Dr. Chong Fang
{"title":"Targeting Ultrafast Spectroscopic Insights into Red Fluorescent Proteins","authors":"Dr. Taylor D. Krueger, Dr. Cheng Chen, Prof. Dr. Chong Fang","doi":"10.1002/asia.202300668","DOIUrl":"10.1002/asia.202300668","url":null,"abstract":"<p>Red fluorescent proteins (RFPs) represent an increasingly popular class of genetically encodable bioprobes and biomarkers that can advance next-generation breakthroughs across the imaging and life sciences. Since the rational design of RFPs with improved functions or enhanced versatility requires a mechanistic understanding of their working mechanisms, while fluorescence is intrinsically an ultrafast event, a suitable toolset involving steady-state and time-resolved spectroscopic techniques has become powerful in delineating key structural features and dynamic steps which govern irreversible photoconverting or reversible photoswitching RFPs, and large Stokes shift (LSS)RFPs. The pertinent <i>cis</i>-<i>trans</i> isomerization and protonation state change of RFP chromophores in their local environments, involving key residues in protein matrices, lead to rich and complicated spectral features across multiple timescales. In particular, ultrafast excited-state proton transfer in various LSSRFPs showcases the resolving power of wavelength-tunable femtosecond stimulated Raman spectroscopy (FSRS) in mapping a photocycle with crucial knowledge about the red-emitting species. Moreover, recent progress in noncanonical RFPs with a site-specifically modified chromophore provides an appealing route for efficient engineering of redder and brighter RFPs, highly desirable for bioimaging. Such an effective feedback loop involving physical chemists, protein engineers, and biomedical microscopists will enable future successes to expand fundamental knowledge and improve human health.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10189873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Counter-Anions Rendered Weak-Interactions Perturb the Stability of Tyrosinase-Mimicked Peroxo-Dicopper(II) Active Site: Unraveling Computational Indicators","authors":"Sumangla Arora, Dr. Puneet Gupta","doi":"10.1002/asia.202300688","DOIUrl":"10.1002/asia.202300688","url":null,"abstract":"<p>It has been observed in literature that the stability of tyrosinase-mimicked μ-η<sup>2</sup>:η<sup>2</sup>-peroxo-dicopper(II) (<b>P</b>) can be perturbed in presence of counter-anions (<b>CA</b>s) such as PhCO<sub>2</sub><sup>−</sup>, CF<sub>3</sub>SO<sub>3</sub><sup>−</sup>, TsO<sup>−</sup> and SbF<sub>6</sub><sup>−</sup>. In this work, we unravel computational indicators using density functional theory to screen and study the stability of <b>P</b> in experimentally-reported cases. These indicators are Gibbs energies, geometrical parameters such as distances and angles, independent gradient model based on Hirshfeld partition (IGMH) generated data, orbitals’ overlap, and distortion-interaction (DI) energies. Our DFT computed Gibbs energies indicate that <b>P</b> is stable in case of PhCO<sub>2</sub><sup>−</sup> and TsO<sup>−</sup>. CF<sub>3</sub>SO<sub>3</sub><sup>−</sup> allows <b>P</b> and its isoelectronic species bis-μ-oxo-dicopper (<b>O</b>) to coexist. SbF<sub>6</sub><sup>−</sup> shows that <b>O</b> is in excess. Our indicators reveal that the stability of <b>P</b> in case of PhCO<sub>2</sub><sup>−</sup> and TsO<sup>−</sup> is due to the better placing of <b>P</b> and its <b>CA</b>, thus leading to better interactions and overlap of orbitals. Other indicator displays that the plane of Cu<sub>2</sub>O<sub>2</sub> core in <b>P</b> is more bend in PhCO<sub>2</sub><sup>−</sup> and TsO<sup>−</sup> cases as compared to the plane in the other two cases. In addition, the IGMH-based indicator displays higher values in the case of PhCO<sub>2</sub><sup>−</sup> and TsO<sup>−</sup> than the other <b>CA</b>s.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10336384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dr. Hao-Yuan Liu, Dr. Zhen-Yu Zhang, Dr. Yi-Ke Zhou, Prof. Dr. Jia-Hua Chen, Prof. Dr. Zhen Yang, Dr. Yuan-He Li
{"title":"Synthesis towards Phainanoid F: Photo-induced 6π-Electrocyclization for Constructing Contiguous All-Carbon Quaternary Centers","authors":"Dr. Hao-Yuan Liu, Dr. Zhen-Yu Zhang, Dr. Yi-Ke Zhou, Prof. Dr. Jia-Hua Chen, Prof. Dr. Zhen Yang, Dr. Yuan-He Li","doi":"10.1002/asia.202300622","DOIUrl":"10.1002/asia.202300622","url":null,"abstract":"<p>In this paper, we report an efficient strategy for synthesizing the DEFGH rings of phainanoid F. The key to the construction of the 13,30-cyclodammarane skeleton of the molecule was a photo-induced 6π-electrocyclization and a homoallylic elimination. Notably, this is a rare example of using electrocyclization reaction to simultaneously construct two vicinal quaternary carbons in total synthesis. The strategy outlined here forms the basis of our total synthesis of Phainanoid F, and it could also serve as a generally applicable approach for synthesizing other natural products containing similar 13,30-cyclodammarane skeletons.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10220524","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Easy Access to Tertiary Amines from Carbonyl Compounds with Substituted Amine-Boranes: A Substrate, Catalyst, and Additive-Free Approach Under Mild Conditions","authors":"Deep Chowdhury, Dr. Arup Mukherjee","doi":"10.1002/asia.202300661","DOIUrl":"10.1002/asia.202300661","url":null,"abstract":"<p>Tertiary amines are ubiquitous and play an essential role in organocatalysis, pharmaceuticals, and fine chemicals. Amongst various synthetic procedures known for their synthesis, the reductive amination of carbonyl compounds has been found to be a proficient method. Over the past few decades, different synthetic strategies for reductive amination have been developed. Most of them suffer from the use of transition metals and/or harsh reaction conditions. Herein, we present an efficient, operationally simple protocol for the chemoselective transformation of carbonyl compounds to tertiary amines under benign conditions. The strategy encompasses a broad substrate scope under the metal-free condition at room temperature and does not require any solvent. A detailed mechanistic investigation was performed with the aid of control experiments and computational study to shed light on the reaction pathway.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10164950","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Deepsagar Manikpuri, Raman Vijaya Sankar, Prof. Dr. Chidambaram Gunanathan
{"title":"Direct Synthesis of Aldoximes: Ruthenium-Catalyzed Coupling of Alcohols and Hydroxylamine Hydrochloride","authors":"Deepsagar Manikpuri, Raman Vijaya Sankar, Prof. Dr. Chidambaram Gunanathan","doi":"10.1002/asia.202300678","DOIUrl":"10.1002/asia.202300678","url":null,"abstract":"<p>A catalytic method for the direct synthesis of oximes from alcohols and hydroxyl amine hydrochloride salt is reported. The reaction is catalyzed by a ruthenium pincer catalyst, which oxidizes alcohols involving amine-amide metal-ligand cooperation, and the in situ formed aldehydes condense with hydroxyl amine to deliver the oximes. Notably, the reaction requires only a catalyst and base; water and liberated hydrogen are the only byproducts, making this protocol attractive and environmentally benign.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10604778","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yongquan Zhang, Tao Ding, Jingshun Wang, Anquan Yao, Changhai Zhang, Tiandong Zhang, Yue Zhang, Yu Feng, Qingguo Chi
{"title":"Improvements in the Electrochemical Performance of Sodium Manganese Oxides by Ti Doping for Aqueous Mg-Ion Batteries","authors":"Yongquan Zhang, Tao Ding, Jingshun Wang, Anquan Yao, Changhai Zhang, Tiandong Zhang, Yue Zhang, Yu Feng, Qingguo Chi","doi":"10.1002/asia.202300542","DOIUrl":"10.1002/asia.202300542","url":null,"abstract":"<p>In recent times, the research on cathode materials for aqueous rechargeable magnesium ion battery has gained significant attention. The focus is on enhancing high-rate performance and cycle stability, which has become the primary research goal. Manganese oxide and its derived Na−Mn−O system have been considered as one of the most promising electrode materials due to its low cost, non-toxicity and stable spatial structure. This work uses hydrothermal method to prepare titanium gradient doped nano sodium manganese oxides, and uses freeze-drying technology to prepare magnesium ion battery cathode materials with high tap density. At the initial current density of 50 mA g<sup>−1</sup>, the NMTO-5 material exhibits a high reversible capacity of 231.0 mAh g<sup>−1</sup>, even at a current density of 1000 mA g<sup>−1</sup>, there is still 122.1 mAh g<sup>−1</sup>. It is worth noting that after 180 cycles of charging and discharging at a gradually increasing current density such as 50–1000 mA g<sup>−1</sup>, it can still return to the original level after returning to 50 mA g<sup>−1</sup>. Excellent electrochemical performance and capacity stability show that NMTO-5 material is a promising electrode material.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10569127","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shivam Pandey, Sabiha Parveen, Prof. Chandra M. R. Volla
{"title":"Rh(II)-Catalyzed Denitrogenative Reaction of N-Sulfonyl-1,2,3-triazoles with Quinolones and Isoquinolones","authors":"Shivam Pandey, Sabiha Parveen, Prof. Chandra M. R. Volla","doi":"10.1002/asia.202300614","DOIUrl":"10.1002/asia.202300614","url":null,"abstract":"<p>Herein, we developed an efficient approach to access biologically relevant 2-aminoquinolines and 1-aminoisoquinolines from readily available <i>N</i>-sulfonyl-1,2,3-triazoles and 2-quinolones or 1-isoquinolones. This transformation involves the selective O−H insertion of these derivatives onto the <i>in situ</i> generated Rh-azavinyl carbenes (Rh-AVC) followed by rearrangement. The reaction proceeds smoothly under operationally simple conditions and the protocol was found to be scalable.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10526166","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dr. Xin Guan, Prof. Yunxing Li, Dr. Hang Jiang, Prof. Ying-Lung Steve Tse, Prof. To Ngai
{"title":"Temperature-Responsive Pickering Double Emulsions Stabilized by Binary Microgels","authors":"Dr. Xin Guan, Prof. Yunxing Li, Dr. Hang Jiang, Prof. Ying-Lung Steve Tse, Prof. To Ngai","doi":"10.1002/asia.202300587","DOIUrl":"https://doi.org/10.1002/asia.202300587","url":null,"abstract":"<p>Microgels are excellent emulsifiers that can self-assemble to reduce interfacial tension and form a steric barrier at an oil-water interface. Herein, we report a two-step emulsification approach to prepare oil-in-water-in-oil (O/W/O) Pickering double emulsions through the dispersion of microgels in two immiscible phases. The stabilization mechanism depends on the uneven distribution and adsorption of hydrophilic water-swollen microgels and hydrophobic octanol-swollen microgels on either outer water droplets or inner oil droplets. Our results reveal that binary microgels outperformed single microgels in terms of interfacial tension reduction and emulsion stabilization. Notably, the binary microgel-stabilized Pickering double emulsions show excellent temperature responsiveness owing to the intrinsic thermal sensitivity of microgels. Consequently, the selective and rapid release of encapsulated substances in different phases can be achieved through the adjustment of the ambient temperature.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 19","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/asia.202300587","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"41087617","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Exploring the Divergent Reactivity of Vinyl Radicals Emanating from Alkynes and Thiols via Photoredox Catalysis","authors":"Sourav Kumar, Dr. Bhahwal Ali Shah","doi":"10.1002/asia.202300693","DOIUrl":"10.1002/asia.202300693","url":null,"abstract":"<p>Organic chemistry has seen a surge in visible-light-driven transformations, which offer unique reaction pathways and access to new synthetic possibilities. We aim to provide a comprehensive understanding of state-of-the-art photo-mediated alkyne functionalization, with a focus on the reactive behavior of vinyl radicals. This review outlines our contributions to the field, including developing new methods for forming carbon-carbon and carbon-heteroatom bonds.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":"18 20","pages":""},"PeriodicalIF":4.1,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"10586664","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}