Pub Date : 2024-01-11DOI: 10.1007/s42773-023-00286-y
Abstract
This study has introduced a pioneering methodology by employing biochars as a basic carbocatalyst in the context of multicomponent reactions. Biochars were produced from different manures and organic wastes using the pyrolysis-carbonization process under limited oxygen conditions. The prepared biochars were well characterized using Fourier transform infrared spectroscopy (FT-IR), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Brunauer–Emmett–Teller (BET) analysis, and powder X-ray diffraction (XRD). The chemical characteristics and potentiometric titration analysis provide compelling evidence of the intriguing basicity properties exhibited by the prepared biochars. The pH values, ash content, and potentiometric titration results confirmed the exceptional basicity characteristics of cow manure biochar formed at 600 oC (CB600), establishing it as the most basic carbocatalyst in this study. Encouraged by these initial results, the activity of the biochars as basic carbocatalysts was evaluated in multicomponent synthesis of 4H-benzo[h]chromene and pyranopyrazoles and 600 °C exhibited the most pronounced catalytic performance owing to its superior total basicity. By these findings, it can be asserted that this work introduces the groundbreaking application of biochars as potent basic carbocatalysts for the multicomponent synthesis of structurally diverse heterocycles. Unveiling the vital basic role of biochars will definitely open up new opportunities in organic chemistry and provide salient features for environmentally-friendly chemistry, including easy retrieval, non-toxicity, and widespread accessibility.
Graphical Abstract
摘要 本研究提出了一种开创性的方法,即在多组分反应中使用生物炭作为基本碳催化剂。在有限的氧气条件下,利用热解-碳化过程从不同的粪便和有机废物中制备生物炭。利用傅立叶变换红外光谱(FT-IR)、扫描电子显微镜(SEM)、能量色散 X 射线光谱(EDX)、Brunauer-Emmett-Teller(BET)分析和粉末 X 射线衍射(XRD)对制备的生物炭进行了表征。化学特性和电位滴定分析提供了令人信服的证据,证明制备的生物脆性具有耐人寻味的碱性特性。pH 值、灰分含量和电位滴定结果证实了在 600 oC 下形成的牛粪生物炭(CB600)具有优异的碱性特性,从而使其成为本研究中碱性最强的碳催化剂。受这些初步结果的鼓舞,在 4H-苯并[h]色烯和吡喃并唑的多组分合成中,对生物炭作为碱性碳催化剂的活性进行了评估。通过这些发现,可以断言这项工作开创性地将生物酵母作为强效碱性碳催化剂,用于多组分合成结构多样的杂环。揭示生物炭的重要基础作用必将为有机化学开辟新的机遇,并为环境友好型化学提供显著特点,包括易于回收、无毒性和广泛可得性。 图表摘要
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Iron-carbon micro-electrolysis system is a promising method for promoting electron transfer in nitrate removal. However, many traditional approaches involving simple physical mixing inevitably suffered from the confined iron-carbon contact area and short validity period, leading to the overuse of iron. Here, a ceramsite-loaded microscale zero-valent iron (mZVI) and acidified carbon (AC) coupled-galvanic cell (CMC) was designed to support chemical, autotrophic and heterotrophic denitrification. Long-term experiments were conducted to monitor the nitrogen removal performance of denitrification reactors filled with CMC and thus optimized the denitrification performance by improving fabrication parameters and various operating conditions. The denitrification contributions test showed that the chemical denitrification pathway contributed most to nitrate removal (57.3%), followed by autotrophic (24.6%) and heterotrophic denitrification pathways (18.1%). The microbial analysis confirmed the significant aggregation of related denitrifying bacteria in the reactors, while AC promoted the expression of relevant nitrogen metabolism genes because of accelerated uptake and utilization of iron complexes. Meanwhile, the electrochemical analysis revealed a significantly improved electron transfer capacity of AC compared to pristine carbon. Overall, our study demonstrated the application of a novel mZVI-AC coupled material for effective nitrate removal and revealed the potential impact of CMC in the multipathway denitrification process.