sustainable chemistry

可持续化学
  • 文章类型: Journal Article
    基于降冰片二烯的光开关已成为利用和存储太阳能的有希望的候选人,作为满足日益增长的能源需求的可行解决方案,有着巨大的希望。尽管有潜力,他们的直接光化学转化为所得四环烷烃的有效性有改进的空间,由于(i)中等量子产率,(ii)与太阳光谱的差的重叠和(iii)光化学逆反应。在这里,我们提出了一种通过芳基取代的降冰片二烯的三重态敏化转化来增强此类分子太阳能热能存储(MOST)系统性能的方法。我们的研究结合了深入的光谱分析,辐照实验,和量子力学计算来阐明所得MOST系统的能量传递机制和固有优势。我们在LED和太阳光照射下使用现成的敏化剂证明了显着的量子产率,大大超过那些通过直接激发与更高能量的光子。与传统方法相比,高能产物的光致反反应不起作用,允许在几分钟内进行定量切换。这些结果不仅强调了三重态敏化MOST系统利用多态光开关的高能量存储能力的潜力,而且还可能刺激敏化策略在光化学能量转换中的更广泛使用。
    Norbornadiene-based photoswitches have emerged as promising candidates for harnessing and storing solar energy, holding great promise as a viable solution to meet the growing energy demands. Despite their potential, the effectiveness of their direct photochemical conversion into the resulting quadricyclanes has room for improvement owing to (i) moderate quantum yields, (ii) poor overlap with the solar spectrum and (iii) photochemical back reactions. Herein, we present an approach to enhance the performance of such molecular solar thermal energy storage (MOST) systems through the triplet-sensitized conversion of aryl-substituted norbornadienes. Our study combines deep spectroscopic analyses, irradiation experiments, and quantum mechanical calculations to elucidate the energy transfer mechanism and inherent advantages of the resulting MOST systems. We demonstrate remarkable quantum yields using readily available sensitizers under both LED and solar light irradiation, significantly surpassing those achieved through direct excitation with photons of higher energy. In contrast to the conventional approach, light-induced back reactions of the high-energy products do not play any role, allowing quantitative switching within minutes. These results not only underscore the potential of triplet-sensitized MOST systems to leverage the high energy storage capabilities of multistate photoswitches but they might also stimulate the broader usage of sensitization strategies in photochemical energy conversion.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    碳催化领域,通常由典型的石墨碳质结构描绘,已经成为一个为多种应用量身定做的蓬勃发展的话题。为此,一种新的不含金属的碳催化剂已经从简单的益生元单体,如氨基氰和乙二醛。所得材料表现出优异的性能,作为用于H2生产和CO2增值的光催化剂,从而揭示其实现可持续目标的真正价值。独特的富氧碳质结构已得到详细的表征,这与石墨层状网络一致。所描述的表现在两个主要的社会问题以及C1/C2平台的轻松准备,使这种被忽视的氮氧化物碳催化剂有望用于现实生活中的环境工作。
    The field of carbocatalysis, often portrayed by paradigmatic graphitic carbonaceous structures, has become a booming topic tailored for multiple applications. To this end, a new metal-free carbocatalyst has been constructed from simple prebiotic monomers such as cyanamide and glyoxal. The resulting material shows an excellent performance as photocatalyst for H2 production and CO2 valorization, thus unveiling its real value to tackle sustainable goals. The unique oxygen-rich carbonaceous structure has been characterized in detail, which is consistent with a graphitic layered network. The described performance in two major societal concerns along with a facile preparation from C1/C2 platforms, makes this type of overlooked oxynitride carbocatalysts promising for real-life environmental endeavors.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    N-杂环代表有机化学的主要和独特类别。由于它们重要的化学物质,它们受到了很多关注,生物医学,和工业用途。美国食品和药物管理局(FDA)批准了大约75%的含有N-基杂环的药物,目前在市场上可以买到。N-杂环化合物作为许多天然产物的骨架存在,是构建药物的关键中间体,兽医用品,和农用化学品经常。在N-基杂环化合物中,生物活性N,N-杂环在现代药物发现和开发过程中具有广泛的应用。头孢唑兰(抗生素),奥美拉唑(抗溃疡),enviradine(抗病毒),利罗唑(抗癌),等。,是含有N的重要药物,N-杂环。N的合成,在可持续条件下的杂环化合物是最活跃的领域之一,因为它们具有重要的生理和生物学特性以及合成实用性。当前的研究要求开发更绿色的产品,更便宜,和更温和的合成N的协议,N-杂环化合物通过避免有毒的金属催化剂来拯救大自然,能源的广泛应用,以及过度使用有害物质。纳米催化剂在可持续合成中起着深远的作用,因为它们具有更大的表面积,微小的尺寸,和最少的能源;它们是环保和安全的,并且与常规催化剂相比,它们提供更高的产率和选择性。设计和合成可能有助于对抗癌症的新型生物活性化合物的研究要求越来越高,因为全球死亡的主要原因是癌症。因此,纳米催化剂在一锅法合成生物有效N的重要用途,本文综述了具有抗癌活性的N-杂环。
    N-heterocycles represent a predominant and unique class of organic chemistry. They have received a lot of attention due to their important chemical, biomedical, and industrial uses. Food and Drug Administration (FDA) approved about 75% of drugs containing N-based heterocycles, which are currently available in the market. N-Heterocyclic compounds exist as the backbone of numerous natural products and act as crucial intermediates for the construction of pharmaceuticals, veterinary items, and agrochemicals frequently. Among N-based heterocyclic compounds, bioactive N,N-heterocycles constitute a broad spectrum of applications in modern drug discovery and development processes. Cefozopran (antibiotic), omeprazole (antiulcer), enviradine (antiviral), liarozole (anticancer), etc., are important drugs containing N,N-heterocycles. The synthesis of N,Nheterocyclic compounds under sustainable conditions is one of the most active fields because of their significant physiological and biological properties as well as synthetic utility. Current research is demanding the development of greener, cheaper, and milder protocols for the synthesis of N,N-heterocyclic compounds to save mother nature by avoiding toxic metal catalysts, extensive application of energy, and the excessive use of hazardous materials. Nanocatalysts play a profound role in sustainable synthesis because of their larger surface area, tiny size, and minimum energy; they are eco-friendly and safe, and they provide higher yields with selectivity in comparison to conventional catalysts. It is increasingly demanding research to design and synthesize novel bioactive compounds that may help to combat cancer since the major causes of death worldwide are due to cancer. Hence, the important uses of nanocatalysts for the one-pot synthesis of biologically potent N,N-heterocycles with anticancer activities have been presented in this review.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    化妆品行业现在正在发生变化,或者更确切地说是在生态转型中,配方如面霜,乳液,和化妆用的粉末,皮肤和头发护理不得含有微塑料,现在是这个领域的禁忌词。如今,许多公司正在加强研究和开发工作,以符合最近和未来的立法,这些立法规定消除它们以保护生态系统。新的生态可持续材料的生产目前是一个热门话题,它在价值超过3500亿美元的市场中占据一席之地,在短时间内将达到超过7000亿美元。这篇综述概述了与在化妆品中使用微塑料有关的主要优点和不利问题及其影响,提供对目前用于改善化妆品的感官特性的聚合物材料的性质的洞察。此外,还描述了世界不同地理区域的各种监管限制,这是反思未来方向的问题。最后,用可持续替代品替代微塑料的可能解决方案的前瞻性愿景完成了下一代个人护理产品的图景,以支持化妆品市场的决策。
    The cosmetic industry is now changing or rather having an ecological transition in which formulations such as creams, lotions, and powders for make-up, skin and hair care must not contain microplastics, now a taboo word in this field. Nowadays, many companies are intensifying their research and development work to align with recent and future legislation that provides for their elimination to safeguard the ecosystem. The production of new eco-sustainable materials is currently a hot topic which finds its place in a market worth above 350 billion dollars which will reach more than 700 billion dollars in a short time. This review offers an overview of the main advantages and adverse issues relating to the use of microplastics in cosmetics and of their impact, providing an insight into the properties of the polymeric materials that are currently exploited to improve the sensorial characteristics of cosmetic products. In addition, the various regulatory restrictions in the different geographical areas of the world are also described, which is matter for reflection on future direction. Finally, a prospective vision of possible solutions to replace microplastics with sustainable alternatives complete the picture of the next generation personal care products to support decision-making in the cosmetic marketplace.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    30秒成功!-维蒂希的反应,有机化学中广泛使用的基本反应,能够使用鳞盐将羰基化合物有效转化为烯烃。传统上,细致的反应设置,包括通过鳞盐的去质子化预先形成反应性叶立德物质,对于在经典的基于溶液的条件下实现高产率反应至关重要。在这份报告中,我们提出了在无溶剂和环境条件下超快速机械诱导的Wittig反应的前所未有的方案,通常无需在严格的空气和水分排除条件下进行繁琐的伊立德预形成。在高能球磨条件下,一系列醛和酮与多种鳞盐反应,经常在30秒内获得相应的烯烃。
    30 Seconds to success! - The Wittig reaction, a fundamental and extensively utilized reaction in organic chemistry, enables the efficient conversion of carbonyl compounds to olefins using phosphonium salts. Traditionally, meticulous reaction setup, including the pre-formation of a reactive ylide species via deprotonation of a phosphonium salt, is crucial for achieving high-yielding reactions under classical solution-based conditions. In this report, we present an unprecedented protocol for an ultra-fast mechanically induced Wittig reaction under solvent-free and ambient conditions, often eliminating the need for tedious ylide pre-formation under strict air and moisture exclusion. A range of aldehydes and ketones were reacted with diverse phosphonium salts under high-energy ball milling conditions, frequently giving access to the respective olefins in only 30 seconds.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    这项研究的重点是设计,生态友好型合成,几种新型三足三苯胺衍生物的表征。通过在甘油中与三(4-乙炔基苯基)胺进行官能化芳基碘化物的Sonogashira偶联,一种容易获得的生物衍生溶剂,我们在短时间内实现了目标产物的合成,高达94%,与使用甲苯作为反应介质的标准条件相比,具有持续较低的E因子和降低的成本。目标分子具有D-(π-A)3或D-(π-D)3结构,其中给电子核通过乙炔间隔物连接到三个给电子(D)或接受电子(A)外围芳族亚基。它们的主要光学和电子特性已通过实验和DFT模拟确定,并提出了在能量转换技术中的可能实现,例如发光太阳能集中器(LSC)和钙钛矿太阳能电池(PSC)。
    This study focuses on the design, eco-friendly synthesis, and characterization of several novel three-legged triphenylamine derivatives. By performing Sonogashira couplings of functionalized aryl iodides with tris(4-ethynylphenyl)amine in glycerol, a readily available bio-derived solvent, we achieved the synthesis of target products in short times and high yields, up to 94%, with consistently lower E-factors and reduced costs compared to standard conditions using toluene as the reaction medium. The target molecules possess a D-(π-A)₃ or D-(π-D)₃ structure, where an electron-donating core connects to three electron-donating (D) or electron-accepting (A) peripheral aromatic subunits through an acetylene spacer. Their main optical and electronic properties have been determined experimentally and by DFT simulations and suggest a possible implementation in energy conversion technologies such as luminescent solar concentrators (LSCs) and perovskite solar cells (PSCs).
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    要获得可降解聚烯烃塑料,乙烯(E)和一氧化碳(CO)的非交替共聚生产聚乙烯(PE)与链酮是特别有吸引力的;它仍然存在重大挑战,例如分子量调节(氢响应)和链端基控制(功能末端)。在这项研究中,我们使用后过渡金属催化剂实现了氢控制的E/CO非交替共聚。该过程产生含有所需的非交替链内酮基(1.0-9.3mol%)且具有范围为43-195kDa的可调分子量的线性PE。在这个反应中,H2作为链转移剂,调节聚合物的分子量,形成独特的醛端基并消除常见的烯属端基;CO经历非交替插入PE链,导致酮-PE的严格非交替结构(>99%)。链内酮基的分散掺入保留了PE的整体性能,并使PE易于光降解,其产生具有明确的乙烯基和乙酰基末端的显著较低分子量的聚合物和低聚物。
    To access degradable polyolefin plastic, non-alternating copolymerization of ethylene (E) and carbon monoxide (CO) for producing polyethylene (PE) with in-chain ketones is particularly appealing; however, it still presents significant challenges such as molecular weight modulation (hydrogen response) and chain endgroup control (functional terminal). In this study, we achieved hydrogen-controlled E/CO non-alternating copolymerization using late transition metal catalysts. This process results in linear PEs containing the desired non-alternating in-chain keto groups (1.0-9.3 mol%) and with tunable molecular weights ranging from 43 to 195 kDa. In this reaction, H2 serves as a chain transfer agent, modulating the polymer\'s molecular weight, forming unique aldehyde endgroups and eliminating usual olefinic endgroups; CO undergoes non-alternating insertion into the PE chain, resulting in a strictly non-alternating structure (> 99%) for the keto-PE. The dispersed incorporation of in-chain keto groups retains bulk properties of PE and makes PE susceptible to photodegradation, which produces significantly lower molecular weight polymers and oligomers with unambiguous vinyl and acetyl terminals.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    如何从基于表面活性剂的微乳液(ME)中有效地回收和再利用表面活性剂一直是一个问题,充满挑战,迫切需要解决。为此,开发了pH触发的沉淀-溶解(PTPD)策略。表面活性剂3-(月桂基氨基)丙烷-1-磺酸钠(LMPS)转化为不溶性沉淀物(LMPS的内盐,LMP)与HCl反应后,通过这种方法,基于LMPS的单相MEs完全去乳化,提供可分离的油混合物,水和LMP。无论ME类型如何,都可以有效地检索LMP(~95.3%),然后可以通过与NaOH反应方便地恢复为LMPS。概念上,LMPS的检索(~96.6%),有毒的苯并[a]芘(BaP,〜99.5%)和来自充分乳化的土壤洗脱液的助表面活性剂正丁醇和油相正庚烷(〜97.1%)的混合物可分别使用PTPD策略和蒸馏,其中土壤洗脱剂是使用基于水包油型LMPS的ME作为洗涤剂从BaP污染的土壤的修复中产生的。它揭示了PTPD策略在含有有毒疏水性有机污染物和过量表面活性剂的土壤洗脱液后处理中的前景。
    How to retrieve and reuse surfactants efficiently from surfactant-based microemulsions (MEs) has long been a problem, which is full of challenges and needs to be solved urgently. To this end, a pH-triggered precipitation-dissolution (PTPD) strategy is developed. The surfactant sodium 3-(laurylamino)propane-1-sulfonate (LMPS) transforms into an insoluble precipitate (the inner salt of LMPS, LMP) after reaction with HCl, by which the monophasic LMPS-based MEs demulsified entirely, giving a separable mixture of oil, water and LMP. LMP can be retrieved efficiently (~95.3%) regardless of the ME type, and can then be conveniently restored to LMPS via reactions with NaOH. Conceptually, the retrieval of LMPS (~96.6%), toxic benzo[a]pyrene (BaP, ~99.5%) and a mixture of co-surfactant n-butanol and the oil phase n-heptane (~97.1%) from the sufficiently emulsified soil eluents is achievable by respectively using the PTPD strategy and distillation, wherein the soil eluents were generated from the remediation of BaP-contaminated soil using an oil-in-water LMPS-based ME as washing agent. It reveals a promising future for the PTPD strategy in the post-processing of soil eluents containing toxic hydrophobic organic contaminants and excessive surfactants.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    可持续发展和可持续化学的概念近年来引起了越来越多的关注,对年轻一代非常重要。在这篇观点文章中,我们分享早期职业化学家如何为其学科的可持续转型做出贡献。我们确定他们可以参与促进变革行动的方式。本文并不试图回答有关在可持续发展背景下推动研究和化学创新的最有前途或紧迫领域的问题。相反,我们希望通过展示教育机会来激励和吸引早期职业化学家追求可持续的行动,外展和决策,研究文化和出版,同时强调现有的挑战和主题的复杂性。我们希望通过为全球可持续的未来提供参与的资源和想法来增强早期职业化学家的能力。虽然这篇文章侧重于学生和早期职业化学家,它提供了进一步刺激来自不同背景的科学家参与的见解。
    The concepts of sustainability and sustainable chemistry have attracted increasing attention in recent years, being of great importance to the younger generation. In this Viewpoint Article, we share how early-career chemists can contribute to the sustainable transformation of their discipline. We identify ways in which they can engage to catalyse action for change. This article does not attempt to answer questions about the most promising or pressing areas driving research and chemical innovation in the context of sustainability. Instead, we want to inspire and engage early-career chemists in pursuing sustainable actions by showcasing opportunities in education, outreach and policymaking, research culture and publishing, while highlighting existing challenges and the complexity of the topic. We want to empower early-career chemists by providing resources and ideas for engagement for a sustainable future globally. While the article focuses on students and early-career chemists, it provides insights to further stimulate the engagement of scientists from diverse backgrounds.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

  • 文章类型: Journal Article
    含有氮官能团和包封的铁基活性位点的碳多孔材料已被建议作为能量转化的电催化剂。然而,它们在通过电催化氢化(ECH)氢化有机底物中的应用仍未探索。在这里,我们报告了用适应的退火程序合成的Fe@C:N材料,并作为苯甲醛氢化的电催化剂进行了测试。使用不同浓度的有机物,和电解结合气相色谱法实验,我们证明,有可能将此类体系结构用于不饱和有机物的ECH。电位控制实验表明,在酸性电解质中,ECH法拉第效率>70%是可能的,同时保持醇对频哪醇二聚产物的选择性。对产物形成速率和周转频率(TOF)值的估计表明,相对于碱和贵金属电极,这些碳封装的体系结构可以在酸性电解质中实现竞争性能。
    Carbon porous materials containing nitrogen functionalities and encapsulated iron-based active sites have been suggested as electrocatalysts for energy conversion, however their applications to the hydrogenation of organic substrates via electrocatalytic hydrogenation (ECH) remain unexplored. Herein, we report on a Fe@C:N material synthesized with an adapted annealing procedure and tested as electrocatalyst for the hydrogenation of benzaldehyde. Using different concentrations of the organic, and electrolysis coupled to gas chromatography experiments, we demonstrate that it is possible to use such architectures for the ECH of unsaturated organics. Potential control experiments show that ECH faradaic efficiencies >70% are possible in acid electrolytes, while maintaining selectivity for the alcohol over the pinacol dimerization product. Estimates of product formation rates and turnover frequency (TOF) values suggest that these carbon-encapsulated architectures can achieve competitive performance in acid electrolytes relative to both base and precious metal electrodes.
    导出

    更多引用

    收藏

    翻译标题摘要

    我要上传

    求助全文

公众号