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Efficient Toluene Degradation using Bacillus subtilis Biofilm Supported Mn-Ce/Zeolite Catalysts 利用枯草芽孢杆菌生物膜支撑的锰-铈/沸石催化剂高效降解甲苯
Pub Date : 2024-02-05 DOI: 10.1016/j.gresc.2024.01.006
Muhammad Zubair Mohsin, Ali Mohsin, Waqas Qamar Zaman, Xiaojuan Zhu, Xihua Zhao, Zain Abbas, Muhammad Hammad Hussain, Ali Shan, Salim ur-Rehman, Muhammad Asif Nawaz, Rabia Omer, Yingping Zhuang, Meijin Guo, Jiaofang Huang

This study investigated a new approach for synthesizing Bacillus subtilis biofilm-supported Mn-Ce/Zeolite catalysts for the degradation of gaseous toluene. Four different metal oxide nano-catalysts (ZMn, ZMnCe-10%, ZMnCe-20%, and ZMnCe-30%) were synthesized with varying ratios of manganese (Mn) and cerium (Ce) on zeolite nanoparticles. TEM, SEM, XRD, BET, XPS, and EDX mapping were used to examine these four samples, as well as simple zeolite. Based on these analyses, the catalytic activity of the prepared samples ZMn, ZMnCe-10%, ZMnCe-20%, and ZMnCe-30% for the complete oxidation of toluene and toluene intermediate products were tested with Non-thermal plasma (NTP) technology in a dielectric barrier discharge (DBD) reactor. Among all, ZMnCe-20% showed the highest toluene degradation efficiency (89%) at low concentrations (200 ppm) and humidity (>50%). Later, highly efficient and hydrophobic nano-biocatalysts were prepared by combining B. subtilis biofilm wild-type (WT) and engineered B. subtilis biofilm EPS with ZMnCe-20% catalyst. EPS is the main component found in biofilm matrix and plays a key role in influencing properties such as biofilm stability, electron transfer, surface roughness and hydrophobicity. Compared to WT B. subtilis biofilm, EPS overexpressed B. subtilis biofilm showed stronger growth and development on ZMnCe-20% nanocatalyst. Moreover, the NTP system packed with ZMnCe-20%/biofilm (EPS+) nano-biocatalyst exhibited the highest toluene degradation activity (99%) with (83%) CO2 selectivity, (up to 50%) reduction in NOx concentration and complete ozone decomposition at (250 ppm) toluene concentrations and increased humidity (>90%). High-energy electrons generated in the NTP system break the C-H and C-C bond between the rings of the toluene molecule, forming several byproducts which are later reacted with active radical species such as O•, OH•, and O3 and further converted into final degradation products (CO2 and H2O). The results demonstrated successful biofilm development and growth on the ZMnCe-20% catalyst with advanced features such as superhydrophobicity, H2O resistance, improved surface roughness, and electron generation. In short, the study's approach combines bioengineering and material science to develop sustainable nano-biocatalysts for removing VOCs in industrial and environmental settings.

本研究探讨了一种合成枯草芽孢杆菌生物膜支撑的锰-铈/沸石催化剂以降解气态甲苯的新方法。在沸石纳米颗粒上以不同的锰(Mn)和铈(Ce)比例合成了四种不同的金属氧化物纳米催化剂(ZMn、ZMnCe-10%、ZMnCe-20% 和 ZMnCe-30%)。利用 TEM、SEM、XRD、BET、XPS 和 EDX 图谱对这四种样品以及简单的沸石进行了研究。根据这些分析,在介质阻挡放电(DBD)反应器中采用非热等离子体(NTP)技术测试了制备的 ZMn、ZMnCe-10%、ZMnCe-20% 和 ZMnCe-30% 样品在完全氧化甲苯和甲苯中间产物方面的催化活性。其中,ZMnCe-20% 在低浓度(200 ppm)和湿度(50%)条件下的甲苯降解效率最高(89%)。随后,将枯草芽孢杆菌生物膜野生型(WT)和工程型枯草芽孢杆菌生物膜 EPS 与 ZMnCe-20% 催化剂结合,制备出高效疏水性纳米生物催化剂。EPS 是生物膜基质中的主要成分,在影响生物膜稳定性、电子传递、表面粗糙度和疏水性等特性方面起着关键作用。与 WT 枯草芽孢杆菌生物膜相比,过表达 EPS 的枯草芽孢杆菌生物膜在 ZMnCe-20% 纳米催化剂上表现出更强的生长和发育能力。此外,装有 ZMnCe-20%/ 生物膜(EPS+)纳米生物催化剂的 NTP 系统在甲苯浓度(250 ppm)和湿度增加(90%)的情况下,甲苯降解活性最高(99%),二氧化碳选择性(83%),氮氧化物浓度降低(高达 50%),臭氧分解完全。NTP 系统中产生的高能电子会打断甲苯分子环间的 C-H 和 C-C 键,形成多种副产品,这些副产品随后会与 O-、OH- 和 O3 等活性自由基物种发生反应,并进一步转化为最终降解产物(CO2 和 H2O)。研究结果表明,ZMnCe-20% 催化剂具有超疏水、抗 H2O、改善表面粗糙度和电子生成等先进特性,可成功实现生物膜的发育和生长。总之,该研究方法结合了生物工程和材料科学,开发出了可持续的纳米生物催化剂,用于去除工业和环境中的挥发性有机化合物。
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引用次数: 0
1,7-Hydride transfer-involved dearomatization of quinolines to access C3-spiro hydroquinolines 1,7-肼基转移参与的喹啉脱芳烃化反应生成 C3-螺氢喹啉
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2024.01.008
Da-Ying Shao, Bin Qiu, Zi-Kang Wang, Zhen-Yuan Liu, Jian Xiao, Xiao-De An
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引用次数: 0
Sustainable electrochemical dearomatization for the synthesis of diverse 2, 3-functionalized indolines 用可持续的电化学脱芳烃法合成多种 2,3- 官能化吲哚啉
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2022.10.009
Jun Chen, Rong Zhang, Caiyan Ma, Peng Zhang, Yonghong Zhang, Bin Wang, Fei Xue, Weiwei Jin, Yu Xia, Chenjiang Liu

Herein, we achieved a green and efficient dearomatization for the synthesis of 2,3-functionalized polycyclic indolines in an electrochemical way. This avoiding of external oxidants and metals approach allowed various nucleophilic sources (Nu ​= ​anilines, TMSN3 and ROH) to perform the products, representing an environmentally benign means. Additionally, the continuous flow electrosynthesis and synthetic transformations also reveal the strong practicality of electrochemistry in organic synthesis.

在此,我们通过电化学方法实现了一种绿色高效的脱芳烃法,用于合成 2,3 官能化多环吲哚啉。这种避免使用外部氧化剂和金属的方法允许各种亲核源(Nu = 苯胺、TMSN3 和 ROH)进行产物合成,是一种对环境无害的方法。此外,连续流电合成和合成转化也揭示了电化学在有机合成中的强大实用性。
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引用次数: 0
Photocatalytic generation of 1,4-disubstituted 1,2,3-triazoles under metal, oxidant and azide-free conditions 在无金属、氧化剂和叠氮化物条件下光催化生成 1,4-二取代的 1,2,3-三唑
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2023.05.001
Changhong Liu, Dilshat Abdukerem, Wenli Zhu, Kun Xia, Zechuan Mao, Ablimit Abdukader

Available online A mild and efficient photocatalytic-induced radical method has been developed for [4 ​+ ​1] cycloaddition reaction of 1,4-disubstituted 1,2,3-triazoles with N-tosylhydrazides and primary amines. The reaction is catalyzed by 20 ​mol% of I2 under metal, azide and oxidant-free conditions. The method is based upon the photocatalytic generation of allyl-type radicals, followed by the iodine-catalyzed production of azoalkenes, which react rapidly with various anilines.

在线提供 一种温和高效的光催化诱导自由基方法已被开发出来,用于 1,4 二取代的 1,2,3 三唑与 N-对甲苯磺酰肼和伯胺的 [4 + 1] 环加成反应。该反应在无金属、叠氮化物和氧化剂的条件下,由 20 mol% 的 I2 催化。该方法以光催化生成烯丙基自由基为基础,然后在碘催化下生成偶氮烯,并迅速与各种苯胺发生反应。
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引用次数: 0
Visible-light-enabled multicomponent synthesis of trifluoromethylated 3-indolequinoxalin-2(1H)-ones without external photocatalysis 无需外部光催化,利用可见光多组分合成三氟甲基化 3-吲哚喹喔啉-2(1H)-酮
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2022.08.002
Letian Zhang , Kai Zheng , Pengfei Zhang , Min Jiang , Jiabin Shen , Chao Chen , Chao Shen

A novel and sustainable visible-light-enabled multicomponent reaction involving quinoxalin-2(1H)-ones, indoles, and CF3SO2Na that does not require an external photocatalyst is described. This photoinduced reaction employs air as the sole oxidant, thereby providing a green and highly step-efficient approach to a series of biologically important trifluoromethylated 3-indolequinoxalin-2(1H)-ones.

本研究描述了一种无需外加光催化剂的新型可持续可见光多组分反应,该反应涉及喹喔啉-2(1H)-酮、吲哚和 CF3SO2Na。这种光诱导反应采用空气作为唯一的氧化剂,从而为一系列具有重要生物意义的三氟甲基化 3-吲哚喹喔啉-2(1H)-酮的制备提供了一种绿色、高效的方法。
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引用次数: 0
Spirooxindoles: Recent report of green synthesis approach 螺吲哚:绿色合成方法的最新报告
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2023.08.001
Agus Rimus Liandi , Antonius Herry Cahyana , Diva Naufal Alfariza , Rahma Nuraini , Renita Wulan Sari , Tio Putra Wendari

Spirooxindole is a compound with a unique framework and broad bioactivities in medicine. In this study, we have reviewed various approaches or methods in synthesizing spirooxindole derivatives focused on green synthesis. Synthesis of spirooxindoles is mainly carried out through multicomponent reactions combined with various green approaches such as the use of heterogeneous catalysts (nano-sized, magnetic, metal-complex, and metal-organic framework catalysts), deep eutectic solvent, solvent-free reactions, catalyst-free reactions, as well as the use of ultrasonic and microwaves irradiation. The green method is carried out in addition to obtaining high yields, it also offers reductions in the use of hazardous chemicals, energy use, purification processes, and waste generation. As a result, green synthesis methods in the synthesis of spirooxindole derivatives are more environmentally friendly.

螺吲哚是一种具有独特结构和广泛生物活性的医药化合物。在本研究中,我们以绿色合成为重点,综述了合成螺氧化吲哚衍生物的各种途径或方法。螺吲哚的合成主要通过多组分反应结合各种绿色方法进行,如使用异相催化剂(纳米级、磁性、金属络合物和金属有机框架催化剂)、深共晶溶剂、无溶剂反应、无催化剂反应以及使用超声波和微波辐照。绿色方法除了能获得高产率外,还能减少有害化学品的使用、能源消耗、净化过程和废物的产生。因此,合成螺吲哚衍生物的绿色合成方法更加环保。
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引用次数: 0
Metal-free and visible-light-mediated method enables the synthesis of olefins from ketones 通过无金属和可见光介导的方法从酮合成烯烃
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2024.02.001
Yu Zhang, Xinyu Han, Rong Wu, Jinxin Wang, Qiannan Li, Jingchuan Lin, Dingding Xia, Xin Hong, Shoubhik Das, Wei-Dong Zhang
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引用次数: 0
Visible-light-induced decarboxylative alkynylation of carboxylic acids in batch and continuous flow 可见光诱导的间歇式和连续式羧酸脱羧炔化反应
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2022.10.002
Longzhou Qin , Xinpeng Zhang , Hao Sun , Xiu Duan , Jie Liu , Mengyu Wu , Xin Yuan , Jiangkai Qiu , Kai Guo

A green efficient photoredox-catalyzed decarboxylative alkynylation of carboxylic acids with alkynyl bromides has been developed. This broadly applicable protocol is presented wherein α-amino, aliphatic and α-oxy acids are converted into useful alkynylation products. The commercially-available organic photocatalyst 4CzIPN is used as the photocatalyst, organic base DBU is utilized as the base, and DMSO serves as solvent. This strategy features mild conditions, is metal-free, and is environmentally friendly. The batch and continuous-flow protocols described were applied to obtain a broader substrate scope of functionalization (more than 50 examples). Furthermore, we demonstrate that the use of microflow technology enhanced and intensified the reaction process, achieving significantly reduced reaction times (i.e., 10 ​min of residence time).

我们开发出了一种绿色高效的光氧催化羧酸与炔基溴化物的脱羧炔基化反应。该方案具有广泛的适用性,可将α-氨基、脂肪族和α-氧基酸转化为有用的炔化产物。采用市售有机光催化剂 4CzIPN 作为光催化剂,有机碱 DBU 作为碱,DMSO 作为溶剂。该方法条件温和,不含金属,对环境友好。应用所述的间歇式和连续流动式方案,可获得更广泛的功能化基质范围(50 多个实例)。此外,我们还证明了微流技术的使用增强和强化了反应过程,大大缩短了反应时间(即 10 分钟的停留时间)。
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引用次数: 0
Thioamide construction via sulfur interrupted Brook rearrangement 通过硫中断布鲁克重排构建硫代酰胺
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2024.02.006
Shunmin Zhang, Yanyan Liao, Xuefeng Jiang
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引用次数: 0
1,7-Hydride transfer-involved dearomatization of quinolines to access C3-spiro hydroquinolines 1,7-肼基转移参与的喹啉脱芳烃化反应生成 C3-螺氢喹啉
Pub Date : 2024-02-01 DOI: 10.1016/j.gresc.2024.01.008
Da-Ying Shao, Bin Qiu, Zi-Kang Wang, Zhen-Yuan Liu, Jian Xiao, Xiao-De An
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引用次数: 0
期刊
Green Synthesis and Catalysis
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