Precision ChemistryPub Date : 2025-01-10eCollection Date: 2025-02-24DOI: 10.1021/prechem.4c00084
Yang Liu, Ziren Wang, Guoliang Hu, Xiaomeng Chen, Ke Xu, Yuqiao Guo, Yi Xie, Changzheng Wu
{"title":"Precision Intercalation of Organic Molecules in 2D Layered Materials: From Interface Chemistry to Low-Dimensional Physics.","authors":"Yang Liu, Ziren Wang, Guoliang Hu, Xiaomeng Chen, Ke Xu, Yuqiao Guo, Yi Xie, Changzheng Wu","doi":"10.1021/prechem.4c00084","DOIUrl":"10.1021/prechem.4c00084","url":null,"abstract":"<p><p>The past few decades have witnessed significant development in intercalation chemistry research aimed at precisely controlling material properties. Intercalation, as a powerful surface and interface synthesis strategy, facilitates the insertion of external guests into van der Waals (vdW) gaps in two-dimensional (2D) layered materials, inducing various modulation effects (the weakening of interlayer interactions, changes in electronic structures, interfacial charge transfer, and symmetry manipulation) to tailor material properties while preserving intralayer covalent bonds. Importantly, benefiting from the very diverse structures and properties of organic molecules, their intercalation enables the integration of various molecules with a wide array of 2D materials, resulting in the creation of numerous organic-inorganic hybrid superlattices with exotic properties, which brings extensive potential applications in fields such as spintronics, superconductor electronics, optoelectronics, and thermoelectrics. Herein, based on recent advancements in organic intercalation systems, we briefly discuss a summary and classification of various organic guest species. We also discuss three modulation effects induced by organic intercalation and further introduce intriguing modulations in physicochemical properties, including superconductivity, magnetism, thermoelectricity and thermal conductivity, chiral-induced spin selectivity (CISS) effects, and interlayer-confined chemical reaction. Finally, we offer insights into future research opportunities and emerging challenges in organic intercalation systems.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 2","pages":"51-71"},"PeriodicalIF":0.0,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11863159/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143524569","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2025-01-09DOI: 10.1021/prechem.4c0008710.1021/prechem.4c00087
Piracha Sanwal, Xinrui Gu, Yifei Zhang* and Gao Li*,
{"title":"The Tiara Nickel Cluster Story from Theory to Catalytic Applications","authors":"Piracha Sanwal, Xinrui Gu, Yifei Zhang* and Gao Li*, ","doi":"10.1021/prechem.4c0008710.1021/prechem.4c00087","DOIUrl":"https://doi.org/10.1021/prechem.4c00087https://doi.org/10.1021/prechem.4c00087","url":null,"abstract":"<p >As a transition material between bulk materials and individual atoms, nickel clusters have interesting electrical and structural characteristics that could make them useful as catalysts. To examine the catalytic efficiency of nickel clusters in different applications, this Review combines experimental techniques with density functional theory (DFT). Researchers have shown that nickel clusters can activate and alter tiny molecules like CO, NO, and H<sub>2</sub> through DFT studies that delve deeply into their electronic structures, adsorption mechanisms, and stability. These findings lay the groundwork for the development of effective catalysts for various processes. Nickel clusters considerably improve the hydrogen evolution reaction (HER), indicating their promise for renewable energy conversion. Furthermore, electrocatalysis for the oxygen evolution reaction (OER) showcases the electrochemical performance of nickel clusters, demonstrating their stability and efficiency. The adaptability of nickel clusters is further demonstrated by their use in nitrogen reduction to ammonia. Experimental data confirm that these clusters are good catalysts for this crucial industrial activity. Hydrocarbon reforming and pollutant degradation are two areas in which research has shown that nickel clusters can be useful in thermal reactions. X-ray absorption spectroscopy (XAS) and environmental transmission electron microscopy (ETEM) are examples of in situ characterization techniques that support theoretical predictions by providing real-time insights into the structural alterations and active sites of nickel clusters during these processes. Preparing the way for future research and practical applications in energy and environmental technologies, this thorough study highlights the great potential of nickel clusters in constructing sustainable and efficient catalytic systems.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 4","pages":"157–171 157–171"},"PeriodicalIF":0.0,"publicationDate":"2025-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00087","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878326","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2025-01-08eCollection Date: 2025-03-24DOI: 10.1021/prechem.4c00081
Er-Fei Zhen, Bing-Yu Liu, Meng-Ke Zhang, Lu Lu Zhang, Chen-Yu Zhang, Jun Cai, Marko M Melander, Jun Huang, Yan-Xia Chen
{"title":"Disentangling Multiple pH-Dependent Factors on the Hydrogen Evolution Reaction at Au(111).","authors":"Er-Fei Zhen, Bing-Yu Liu, Meng-Ke Zhang, Lu Lu Zhang, Chen-Yu Zhang, Jun Cai, Marko M Melander, Jun Huang, Yan-Xia Chen","doi":"10.1021/prechem.4c00081","DOIUrl":"10.1021/prechem.4c00081","url":null,"abstract":"<p><p>Understanding how the electrolyte pH affects electrocatalytic activity is a topic of crucial importance in a large variety of systems. However, unraveling the origin of the pH effects is complicated often by the fact that both the reaction driving forces and reactant concentrations in the electric double layer (EDL) change simultaneously with the pH value. Herein, we employ the hydrogen evolution reaction (HER) at Au(111)-aqueous solution interfaces as a model system to disentangle different pH-dependent factors. In 0.1 M NaOH, the HER current density at Au(111) in the potential range of -0.4 V < <i>E</i> <sub>RHE</sub> < 0 V is up to 60 times smaller than that in 0.1 M HClO<sub>4</sub>. A reaction model with proper consideration of the local reaction conditions within the EDL is developed. After correcting for the EDL effects, the rate constant for HER is only weakly pH-dependent. Our analysis unambiguously reveals that the observed pH effects are mainly due to the pH-dependent reorganization free energy, which depends on the electrostatic potential and the local reaction conditions within the EDL. Possible origins of the pH and temperature dependence of the activation energy and the electron transfer coefficients are discussed. This work suggests that factors influencing the intrinsic pH-dependent kinetics are easier to understand after proper corrections of EDL effects.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"135-148"},"PeriodicalIF":0.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11938166/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143731914","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2025-01-08DOI: 10.1021/prechem.4c0008110.1021/prechem.4c00081
Er-Fei Zhen, Bing-Yu Liu, Meng-Ke Zhang, Lu−Lu Zhang, Chen-Yu Zhang, Jun Cai, Marko M. Melander, Jun Huang* and Yan-Xia Chen*,
{"title":"Disentangling Multiple pH-Dependent Factors on the Hydrogen Evolution Reaction at Au(111)","authors":"Er-Fei Zhen, Bing-Yu Liu, Meng-Ke Zhang, Lu−Lu Zhang, Chen-Yu Zhang, Jun Cai, Marko M. Melander, Jun Huang* and Yan-Xia Chen*, ","doi":"10.1021/prechem.4c0008110.1021/prechem.4c00081","DOIUrl":"https://doi.org/10.1021/prechem.4c00081https://doi.org/10.1021/prechem.4c00081","url":null,"abstract":"<p >Understanding how the electrolyte pH affects electrocatalytic activity is a topic of crucial importance in a large variety of systems. However, unraveling the origin of the pH effects is complicated often by the fact that both the reaction driving forces and reactant concentrations in the electric double layer (EDL) change simultaneously with the pH value. Herein, we employ the hydrogen evolution reaction (HER) at Au(111)-aqueous solution interfaces as a model system to disentangle different pH-dependent factors. In 0.1 M NaOH, the HER current density at Au(111) in the potential range of −0.4 V < <i>E</i><sub>RHE</sub> < 0 V is up to 60 times smaller than that in 0.1 M HClO<sub>4</sub>. A reaction model with proper consideration of the local reaction conditions within the EDL is developed. After correcting for the EDL effects, the rate constant for HER is only weakly pH-dependent. Our analysis unambiguously reveals that the observed pH effects are mainly due to the pH-dependent reorganization free energy, which depends on the electrostatic potential and the local reaction conditions within the EDL. Possible origins of the pH and temperature dependence of the activation energy and the electron transfer coefficients are discussed. This work suggests that factors influencing the intrinsic pH-dependent kinetics are easier to understand after proper corrections of EDL effects.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"135–148 135–148"},"PeriodicalIF":0.0,"publicationDate":"2025-01-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00081","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675855","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Boosting Turnover in the Triarylborane-Catalyzed Hydrogenation of <i>N</i>-Substituted Indoles via Olefin-to-Nitrogen Lewis Base Switching in H<sub>2</sub>-Cleavage Steps.","authors":"Taiki Hashimoto, Masakazu Tanigawa, Kimitaka Kambe, Sensuke Ogoshi, Yoichi Hoshimoto","doi":"10.1021/prechem.4c00090","DOIUrl":"10.1021/prechem.4c00090","url":null,"abstract":"<p><p>The shelf-stable heteroleptic borane B(2,6-Cl<sub>2</sub>C<sub>6</sub>H<sub>3</sub>)(3,5-Br<sub>2</sub>-2,6-F<sub>2</sub>C<sub>6</sub>H)<sub>2</sub> (<b>B</b> <sup><b>7</b></sup> ) efficiently catalyzes the solvent-free hydrogenation of various substituted indoles to indolines with an unprecedented turnover number of 8,500, which is more than 400-fold higher than that reported for B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub> under diluted conditions. Mechanistic studies revealed that this hydrogenation proceeds via an olefin-to-nitrogen switching of Lewis bases involved in the H<sub>2</sub>-cleavage steps: initially, H<sub>2</sub> cleavage is mediated by a frustrated Lewis pair (FLP) comprising the indole C3-carbon and boron atoms, which then switches to an FLP system comprising the indoline nitrogen and boron atoms after formation of the indoline. This study demonstrates the potential of relatively benign main-group elements for the catalytic synthesis of valuable N-containing molecules using H<sub>2</sub>.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"128-134"},"PeriodicalIF":0.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11938162/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143731911","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2024-12-18DOI: 10.1021/prechem.4c0007410.1021/prechem.4c00074
Jung Yeon Park, Dongjun Baek, Hyunggeun Min, Bongjun Yeom, Jeong Sook Ha and Yongju Kim*,
{"title":"Aromatic Anion Carrier via Self-Assembly with Imidazolium-Fused Aromatic Amphiphiles","authors":"Jung Yeon Park, Dongjun Baek, Hyunggeun Min, Bongjun Yeom, Jeong Sook Ha and Yongju Kim*, ","doi":"10.1021/prechem.4c0007410.1021/prechem.4c00074","DOIUrl":"https://doi.org/10.1021/prechem.4c00074https://doi.org/10.1021/prechem.4c00074","url":null,"abstract":"<p >The transport of anions across cell membranes is difficult because of the negatively charged outer surfaces of cell membranes. To overcome this limitation, herein, we report a system for transporting aromatic anions across cellular membranes via self-assembly using a synthetic imidazolium-fused aromatic amphiphile. The amphiphile with cationic and aromatic groups in close proximity to each other could interact with anionic pyranine via electrostatic and aromatic interactions to form supramolecular vesicles. Supramolecular vesicles based on the synthetic imidazolium-fused aromatic amphiphile and pyranine complex transport anionic aromatic pyranine across the membranes of live MCF-7 cells without cytotoxicity.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 4","pages":"214–220 214–220"},"PeriodicalIF":0.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00074","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143878397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Boosting Turnover in the Triarylborane-Catalyzed Hydrogenation of N-Substituted Indoles via Olefin-to-Nitrogen Lewis Base Switching in H2-Cleavage Steps","authors":"Taiki Hashimoto, Masakazu Tanigawa, Kimitaka Kambe, Sensuke Ogoshi and Yoichi Hoshimoto*, ","doi":"10.1021/prechem.4c0009010.1021/prechem.4c00090","DOIUrl":"https://doi.org/10.1021/prechem.4c00090https://doi.org/10.1021/prechem.4c00090","url":null,"abstract":"<p >The shelf-stable heteroleptic borane B(2,6-Cl<sub>2</sub>C<sub>6</sub>H<sub>3</sub>)(3,5-Br<sub>2</sub>-2,6-F<sub>2</sub>C<sub>6</sub>H)<sub>2</sub> (<b>B</b><sup><b>7</b></sup>) efficiently catalyzes the solvent-free hydrogenation of various substituted indoles to indolines with an unprecedented turnover number of 8,500, which is more than 400-fold higher than that reported for B(C<sub>6</sub>F<sub>5</sub>)<sub>3</sub> under diluted conditions. Mechanistic studies revealed that this hydrogenation proceeds via an olefin-to-nitrogen switching of Lewis bases involved in the H<sub>2</sub>-cleavage steps: initially, H<sub>2</sub> cleavage is mediated by a frustrated Lewis pair (FLP) comprising the indole C3-carbon and boron atoms, which then switches to an FLP system comprising the indoline nitrogen and boron atoms after formation of the indoline. This study demonstrates the potential of relatively benign main-group elements for the catalytic synthesis of valuable N-containing molecules using H<sub>2</sub>.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"128–134 128–134"},"PeriodicalIF":0.0,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00090","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675725","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2024-12-12DOI: 10.1021/prechem.4c0007510.1021/prechem.4c00075
Naeem Ahmed*, Wei Luo, Ruijuan Zhao, Qiu Zhang, Di Wu, Xia Zheng, Haorui Wang and Chunhua Cui*,
{"title":"Role of Plasma in Catalyst Preparation and Modification for Oxygen Evolution Reaction","authors":"Naeem Ahmed*, Wei Luo, Ruijuan Zhao, Qiu Zhang, Di Wu, Xia Zheng, Haorui Wang and Chunhua Cui*, ","doi":"10.1021/prechem.4c0007510.1021/prechem.4c00075","DOIUrl":"https://doi.org/10.1021/prechem.4c00075https://doi.org/10.1021/prechem.4c00075","url":null,"abstract":"<p >Plasma as a promising solution to catalyst synthesis and modification has received great attention in the field of electrochemical water splitting. However, a comprehensive overview detailing how plasma treatments of catalysts enhance oxygen evolution reaction (OER) performance is currently lacking. Here, we review the advances and challenges in cold plasma for catalyst preparation and modification. We discuss the underlying mechanisms responsible for enhanced OER performance on plasma-treated catalysts, where the surface area, active sites, vacancy type/content, heteroatom doping, etching, and surface functionalization could be mediated. This review aims to provide valuable insights into the role of plasma treatments in advancing OER electrocatalysis for sustainable energy applications.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"110–127 110–127"},"PeriodicalIF":0.0,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/prechem.4c00075","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143675724","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Precision ChemistryPub Date : 2024-12-12eCollection Date: 2025-03-24DOI: 10.1021/prechem.4c00075
Naeem Ahmed, Wei Luo, Ruijuan Zhao, Qiu Zhang, Di Wu, Xia Zheng, Haorui Wang, Chunhua Cui
{"title":"Role of Plasma in Catalyst Preparation and Modification for Oxygen Evolution Reaction.","authors":"Naeem Ahmed, Wei Luo, Ruijuan Zhao, Qiu Zhang, Di Wu, Xia Zheng, Haorui Wang, Chunhua Cui","doi":"10.1021/prechem.4c00075","DOIUrl":"10.1021/prechem.4c00075","url":null,"abstract":"<p><p>Plasma as a promising solution to catalyst synthesis and modification has received great attention in the field of electrochemical water splitting. However, a comprehensive overview detailing how plasma treatments of catalysts enhance oxygen evolution reaction (OER) performance is currently lacking. Here, we review the advances and challenges in cold plasma for catalyst preparation and modification. We discuss the underlying mechanisms responsible for enhanced OER performance on plasma-treated catalysts, where the surface area, active sites, vacancy type/content, heteroatom doping, etching, and surface functionalization could be mediated. This review aims to provide valuable insights into the role of plasma treatments in advancing OER electrocatalysis for sustainable energy applications.</p>","PeriodicalId":29793,"journal":{"name":"Precision Chemistry","volume":"3 3","pages":"110-127"},"PeriodicalIF":0.0,"publicationDate":"2024-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11938164/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143731919","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}