Chemistry methods : new approaches to solving problems in chemistry最新文献_第3页

Accurate Determination of Molecular Sizes of a Solute in Water From its Translational Self-Diffusion Coefficient

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-03 DOI: 10.1002/cmtd.202400063

Francesco Zaccaria, Alceo Macchioni, Cristiano Zuccaccia

{"title":"Accurate Determination of Molecular Sizes of a Solute in Water From its Translational Self-Diffusion Coefficient","authors":"Francesco Zaccaria, Alceo Macchioni, Cristiano Zuccaccia","doi":"10.1002/cmtd.202400063","DOIUrl":"https://doi.org/10.1002/cmtd.202400063","url":null,"abstract":"Determining accurate molecular dimensions in water, from measured translational self-diffusion coefficients (Dt), is extremely important in biochemistry, supramolecular chemistry, organometallic chemistry and beyond, but it still represents a big challenge especially for small and medium-sized molecules. Indeed, current semiempirical adaptations of the Stokes-Einstein equation, which allow accurate determination of molecular size of solutes in organic solvents, proved inadequate for aqueous systems. To overcome such a major limitation, herein, we introduce a novel approach that unlocks the quantitative interpretation of Dt in water. By analyzing ~70 diverse molecules with volumes ranging from 101 Å3 to 103 Å3, and selecting the partial molar radius (rM) as a reliable proxy for the hydrodynamic radius (rH), we derived a semiempirical equation that enables accurate determination of hydrodynamic volume (VH) of solutes in aqueous solutions, effectively accounting for the distinctive hydrogen-bonding properties of water. This approach fills a crucial gap, enhancing precise molecular characterization of polar and non-polar solutes in water.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 5","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400063","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143944873","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}

引用次数: 0

An Efficient Solid-Phase Synthetic Approach to Prepare TACN-Functionalized Peptides

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-03 DOI: 10.1002/cmtd.202400053

Yik-Hoi Yeung, Pak-Lun Lam, Dr. Waygen Thor, Hei-Yui Kai, Tsz-Lam Cheung, Dr. Yue Wu, Prof. Dr. Ga-Lai Law, Prof. Dr. Nicholas J. Long, Prof. Dr. Ka-Leung Wong

引用次数: 0

Physicochemical vs Electrochemical Technologies for Metal Recovery – Main Insights, Comparison, Complementarity and Challenges 金属回收的物理化学与电化学技术——主要见解、比较、互补和挑战

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-02-03 DOI: 10.1002/cmtd.202400046

Stefanos Mourdikoudis, Xochitl Dominguez-Benetton

{"title":"Physicochemical vs Electrochemical Technologies for Metal Recovery – Main Insights, Comparison, Complementarity and Challenges","authors":"Stefanos Mourdikoudis, Xochitl Dominguez-Benetton","doi":"10.1002/cmtd.202400046","DOIUrl":"https://doi.org/10.1002/cmtd.202400046","url":null,"abstract":"The quest toward the development of new, more eco-friendly removal/recycling/recovery methods for a range of valuable elements is intense nowadays. In this Review we present and discuss in a critical way the best available physicochemical processes versus modern electrochemical approaches for metal recovery of elements which form part of spent catalysts or other sources such as wastewater, mining waste and spent batteries. These techniques include coagulation/flocculation, precipitation, electrocoagulation/electroflotation, membrane electrolysis, electrodeposition/electrowinning and gas-diffusion electrocrystallization (GDEx). Several key performance indicators (KPIs) are utilized to facilitate the critical analysis of the different recovery methods. Such indicators have to do, for example, with the efficiency, the cost, the complexity, and the environmental friendliness of the methods used. In some cases, the recovered metals can be further used for specific applications, including the fabrication of electrocatalysts for reactions of interest. When possible, the more novel electrified technologies are benchmarked versus the state-of-the art approaches. This manuscript helps to summarize all types of approaches in a comparative manner. When the targeted metal cannot be recovered by any of the technologies explored, its removal can also be considered as satisfactory in some extent, especially if the element under discussion poses a risk of toxicity for the environment or for human health. Recovery technologies are sometimes combined for an optimum effect, exploiting the advantages of each approach and mitigating their drawbacks. Our review provides also some examples for ‘removal-only’ possibilities of the studied methods, though its primary focus is the metal recovery aiming for metal reuse in the best possible scenarios.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 3","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400046","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581481","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}

引用次数: 0

Sodium-Potassium Competition as a Tool for Chemoselective Cucurbit[n]uril-Xenon Host–Guest Complexation in Imaging Applications 钠钾竞争作为化学选择性葫芦素-氙主-客体络合在成像中的应用

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-28 DOI: 10.1002/cmtd.202400033

Dr. Katarzyna Dziubińska-Kühn, Dr. Guzel Musabirova, Sophie Effertz, Prof. Jörg Matysik, Prof. Renaud Blaise Jolivet

{"title":"Sodium-Potassium Competition as a Tool for Chemoselective Cucurbit[n]uril-Xenon Host–Guest Complexation in Imaging Applications","authors":"Dr. Katarzyna Dziubińska-Kühn, Dr. Guzel Musabirova, Sophie Effertz, Prof. Jörg Matysik, Prof. Renaud Blaise Jolivet","doi":"10.1002/cmtd.202400033","DOIUrl":"https://doi.org/10.1002/cmtd.202400033","url":null,"abstract":"Cucurbit[n]urils (CB[n]) are a family of macromolecules, capable of encapsulating neutral or charged species. Due to their low toxicity, good solubility, and transport properties resulting from the structure forming the cage, they have gained popularity in imaging-oriented studies. In vitro studies have shown that one of the guests compatible with the CB[n] hosts are Xe atoms, leading to high-resolution 129Xe magnetic resonance signals in pulmonary medical imaging. This prompts the question of whether similar results could be achieved in vivo in other tissues and body fluids. Here, we demonstrate how the varying efficacy of Xe encapsulation by a CB[6] cage is governed by the Na+ : K+ molecular ratio in simulated body fluids. Moving from a high concentration of Na+ to an excess of K+ in the solution significantly increases Xe encapsulation by the macromolecules. This finding indicates chemoselectivity of cucurbit[6]uril host-guest interactions. Since Na+ and K+ are the most abundant ions in human body fluids, our results provide a theoretical foundation for future liquid-state in vivo Xe imaging in medical applications.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 3","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400033","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582060","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}

引用次数: 0

Construction of Porous Tetrazine-Functionalized Networks: From Two- to Three-Dimensional Counterparts with Tunable Properties 多孔四嗪功能化网络的构建：从二维到三维对应物的可调性质

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-28 DOI: 10.1002/cmtd.202400042

Dr. Xian Suo, Dr. Juntian Fan, Dr. Liqi Qiu, Dr. Meijia Li, Dr. Bishnu P. Thapaliya, Dr. Chi-Linh Do-Thanh, Dr. Ziyang Lu, Dr. Ilja Popovs, Dr. Shannon M. Mahurin, Dr. Zhenzhen Yang, Dr. Sheng Dai

{"title":"Construction of Porous Tetrazine-Functionalized Networks: From Two- to Three-Dimensional Counterparts with Tunable Properties","authors":"Dr. Xian Suo, Dr. Juntian Fan, Dr. Liqi Qiu, Dr. Meijia Li, Dr. Bishnu P. Thapaliya, Dr. Chi-Linh Do-Thanh, Dr. Ziyang Lu, Dr. Ilja Popovs, Dr. Shannon M. Mahurin, Dr. Zhenzhen Yang, Dr. Sheng Dai","doi":"10.1002/cmtd.202400042","DOIUrl":"https://doi.org/10.1002/cmtd.202400042","url":null,"abstract":"Porous organic networks (PONs) linked by aza-fused rings are extensively studied and demonstrated wide applications in diverse fields. It is a long-term attractive and challenging subject to explore novel PONs functionalized by unexplored aza-fused moieties. Herein, a series of tetrazine-linked PONs (Tz-PONs) were constructed from two-dimensional to three-dimensional counterparts with tunable properties. The reaction pathway composed of the amidrazone intermediates formation using multiply substituted aromatic nitrile monomers was catalyzed by zinc salts with Lewis super acidity in the presence of hydrazine, and the subsequent tetrazine formation was assisted by sodium nitrite solution. Textural property of the as-constructed scaffolds could be tuned by the acidity of the zinc salts, as well as the organic solvents. As an initial assessment, those Tz-PONs displayed different photo absorption behavior, which may influence the corresponding photocatalysis.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 4","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400042","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143793817","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}

引用次数: 0

Operando Luminescence Thermometry of a Solid Catalyst in a Reactor during a High-Temperature Chemical Process 高温化学过程中反应器中固体催化剂的操作发光测温仪

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-21 DOI: 10.1002/cmtd.202400044

Daniël W. Groefsema, Dr. Freddy T. Rabouw, Michiel Boele, Dr. Alexander P. van Bavel, Prof. Dr. Bert M. Weckhuysen

{"title":"Operando Luminescence Thermometry of a Solid Catalyst in a Reactor during a High-Temperature Chemical Process","authors":"Daniël W. Groefsema, Dr. Freddy T. Rabouw, Michiel Boele, Dr. Alexander P. van Bavel, Prof. Dr. Bert M. Weckhuysen","doi":"10.1002/cmtd.202400044","DOIUrl":"https://doi.org/10.1002/cmtd.202400044","url":null,"abstract":"In most catalytic processes, thermal energy is released or consumed locally in a reactor due to the exothermicity or endothermicity of the chemical reactions. This causes the actual operating temperature of the catalyst material to deviate from the reactor temperature, which can lead to underperformance, reduced catalyst stability, or even thermal runaway. Conventional methods to measure the catalyst temperature, with a thermocouple in the reactor oven or in the catalyst bed, suffer from complications because of separation between the sensor and catalyst material, chemical activity of the thermocouple/coating material, added complexity of the setup, and disruption of the reactant flow and heat flow through the catalyst bed. Here, we show the possibilities and challenges of luminescence thermometry as an analytical technique for remote temperature monitoring of the local catalyst temperature in a strongly exothermic high-temperature reaction environment. We observe that the luminescence lifetime depends not only temperature, but also on oxygen concentration, which can introduce a significant systematic error of up to 40 °C in the recorded temperature. In the case of ratiometric luminescence thermometry, this error is strongly reduced to ~5 °C. We use the ratiometric technique to confirm its applicability in the exothermic oxidative coupling of methane (OCM) process at high reaction temperatures, showing an exothermic increase in the local catalyst temperature of up to 100 °C, relative to the constant reactor temperature under inert conditions.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 3","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400044","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582096","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}

引用次数: 0

Optimised Synthesis of Rhombic dodecahedral Cu2O Nanoparticles: A Pathway to Superior Morphological Control 菱形十二面体 Cu2O 纳米粒子的优化合成：实现卓越形态控制的途径

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-21 DOI: 10.1002/cmtd.202400050

Lorenzo Sarasino, Teruhisa Ohno, Maria Cristina Paganini

{"title":"Optimised Synthesis of Rhombic dodecahedral Cu2O Nanoparticles: A Pathway to Superior Morphological Control","authors":"Lorenzo Sarasino, Teruhisa Ohno, Maria Cristina Paganini","doi":"10.1002/cmtd.202400050","DOIUrl":"https://doi.org/10.1002/cmtd.202400050","url":null,"abstract":"Cuprous oxide (Cu2O) nanoparticles hold significant promise for photocatalytic applications due to their narrow bandgap and high surface reactivity. This study focuses on the synthesis of rhombic dodecahedral Cu2O (RD-Cu2O) nanoparticles, totally enclosed by {110} facets, known to exhibit superior photocatalytic performance over the other low-index crystallographic facets. The precise control over the synthesis conditions can significantly enhance the exposure of this highly active face and therefore improve the catalytic performance of Cu2O nanoparticles, making them superior for applications in pollutant degradation, organic reactions, and artificial photosynthesis. We systematically optimised the synthesis parameters, including reactants concentration, pH and other reaction conditions, to achieve a significant scale up of well-defined RD- Cu2O nanoparticles production, strictly necessary for the use of this photocatalyst on a larger scale. The optimised and scaled up synthesis require 2.0 mmol of CuCl2, 6.0 mmol of Sodium dodecyl sulphate (SDS), 9.6 mmol of NH2OH ⋅ HCl and 7.0 mmol of NaOH added in this order to 400 ml of water at 25 °C. The optimised nanoparticles demonstrated a narrow size distribution and a high degree of crystallographic control. Characterisation techniques such as FESEM, XRD, EPR, UV-Vis spectroscopy, and XPS confirmed the improved morphological and structural properties of the synthesised RD-Cu2O nanoparticles.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 4","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400050","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143793808","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}

引用次数: 0

All-in-One Portable Electrochemical Strips for Drug Release, Delivery and Monitoring 用于药物释放、传递和监测的便携式电化学试纸条

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-17 DOI: 10.1002/cmtd.202400079

Sima Singh, Mohga Khater, Ada Raucci, Ovidio Catanzano, Fabiana Quaglia, Stefano Cinti

引用次数: 0

Probing Activation and Deactivation Mechanisms in Electrochemical CO2 Reduction Reaction and Water Splitting through In-Situ/Operando Analysis 利用原位/Operando分析探讨电化学CO2还原反应和水裂解的活化和失活机理

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-17 DOI: 10.1002/cmtd.202400066

Woo Seok Cheon, Jaehyun Kim, Ho Won Jang

{"title":"Probing Activation and Deactivation Mechanisms in Electrochemical CO2 Reduction Reaction and Water Splitting through In-Situ/Operando Analysis","authors":"Woo Seok Cheon, Jaehyun Kim, Ho Won Jang","doi":"10.1002/cmtd.202400066","DOIUrl":"https://doi.org/10.1002/cmtd.202400066","url":null,"abstract":"The transition to a carbon-neutral society demands the development of efficient and durable electrocatalysts to drive electrochemical water splitting and CO2 reduction reactions (CO2RR). To fabricate high-performing electrocatalysts, it is essential to unveil catalyst materials’ activation and deactivation mechanisms under actual reaction conditions, a challenge that ex-situ/post-mortem characterization cannot fulfill. In-situ transmission electron microscopy, X-ray spectroscopy, and Raman spectroscopy, along with various other analytical techniques, are essential methods for revealing the structural and chemical properties of electrochemical catalyst materials in both bulk and surface. In-situ/operando characterization offers unprecedented insights into the structural and electronic changes on catalyst surfaces, revealing critical aspects of catalytic activity, selectivity and stability during operation. These methods are useful in identifying active sites, understanding morphology and phase transitions, and uncovering the underlying mechanisms driving catalytic processes. This perspective explores recent works on the application of in-situ/operando spectroscopic and microscopic techniques to electrochemical CO2RR and water splitting. By organizing recent findings, we highlight the irreplaceable role of in-situ/operando analysis in refining catalyst design for enhanced performance and robustness. Furthermore, we discuss future directions for integrating these characterization methods into catalyst development workflows, offering a roadmap toward developing electrocatalyst materials for green hydrogen production and CO2 reduction.","PeriodicalId":72562,"journal":{"name":"Chemistry methods : new approaches to solving problems in chemistry","volume":"5 6","pages":""},"PeriodicalIF":6.1,"publicationDate":"2025-01-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/cmtd.202400066","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144214114","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}

引用次数: 0

Small Molecule X-ray Crystal Structures at a Crossroads

IF 6.1

Chemistry methods : new approaches to solving problems in chemistry Pub Date : 2025-01-10 DOI: 10.1002/cmtd.202400052

Nathan D. D. Hill, Prof. Dr. René T. Boeré

引用次数: 0