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Greetings from the New Editorial Board Chair 来自编委会新主席的问候
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-15 DOI: 10.1039/D3GC90076B
Javier Pérez-Ramírez introduces himself as the new chair of the editorial board of Green Chemistry.
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引用次数: 0
Magnetic hollow micro-sized nanoaggregates for synergistically accelerating PET glycolysis† 磁空心微纳米聚集体协同加速PET糖酵解†
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-15 DOI: 10.1039/D3GC01762A
Ling-Xia Yun, Yan Wei, Qian Sun, Yu-Ting Li, Bin Zhang, Hang-Tian Zhang, Zhi-Gang Shen and Jie-Xin Wang

Polyethylene terephthalate (PET), as the most widely utilized polyester, causes global environmental problems due to its massive and durable accumulation in natural environments. The glycolysis of PET is an attractive alternative to mechanical recycling, but there remains a strong demand for efficient, convenient, and inexpensive catalysts. Herein, we present a spray-drying-assisted way to construct magnetic hollow micro-sized nanoaggregates (HMNAs) by assembling composite metal oxide nanoparticles to depolymerize PET synergistically. The as-prepared ZnO–Fe3O4 HMNAs completely depolymerized PET with a high monomer yield of 92.3% in a short period of 30 min at 190 °C, far above individual ZnO and Fe3O4 nanoparticles (NPs). The composite HMNAs can be magnetically separated in a few minutes and maintain a high activity for 5 cycles. DFT study reveals that the HMNAs effectively facilitated glycolysis by the high content of Lewis acid sites as well as the stronger adsorption between PET and the catalyst owing to the structural synergy effect of ZnO–Fe3O4 HMNAs. Furthermore, this spray drying strategy as a versatile and scalable methodology is extended to fabricate other HMNAs, exhibiting a similarly enhanced efficiency of glycolysis. The HMNAs are expected to open up avenues for the design of catalysts for upcycling of discarded plastics.

聚对苯二甲酸乙二醇酯(PET)是应用最广泛的一种聚酯,由于其在自然环境中大量且持久的积累,造成了全球性的环境问题。PET的糖酵解是机械回收的一种有吸引力的替代方法,但对高效、方便和廉价的催化剂仍然有很强的需求。在此,我们提出了一种喷雾干燥辅助方法,通过组装复合金属氧化物纳米粒子来协同解聚PET来构建磁性中空微尺度纳米聚集体(HMNAs)。所制备的ZnO - Fe3O4 HMNAs在190℃下,在30 min内完全解聚PET,单体收率高达92.3%,远高于单独的ZnO和Fe3O4纳米颗粒(NPs)。复合hnas可以在几分钟内磁性分离,并保持5个循环的高活性。DFT研究表明,hnas通过高含量的Lewis酸位点有效促进糖酵解,并且由于ZnO-Fe3O4 hnas的结构协同作用,PET与催化剂之间的吸附更强。此外,这种喷雾干燥策略作为一种通用的和可扩展的方法被扩展到制造其他hnas,表现出类似的糖酵解效率的提高。hnas有望为设计废弃塑料升级回收的催化剂开辟道路。
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引用次数: 0
Carbazole-fused coumarin based oxime esters (OXEs): efficient photoinitiators for sunlight driven free radical photopolymerization† 卡巴唑-香豆素基肟酯(OXEs):日光驱动自由基光聚合的高效光引发剂†
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-15 DOI: 10.1039/D3GC02004E
Yijun Zhang, Zheng Liu, Timur Borjigin, Bernadette Graff, Fabrice Morlet-Savary, Michael Schmitt, Didier Gigmes, Frédéric Dumur and Jacques Lalevée

The use of sunlight to initiate free radical polymerization under air is a key challenge. Due to the associated low light intensity, usual or commercial photoinitiators are characterized by a low efficiency. In this work, seventeen carbazole-fused coumarin-based oxime esters were developed as monocomponent and photocleavable (Type I) initiators of polymerization displaying excellent light absorption properties in the visible range. Compared to the benchmark photoinitiator (diphenyl(2,4,6-trimethylbenzoyl)phosphine oxide), some of them (namely OXE-1 and OXE-5) could show photoinitiation performance similar to or better than the reference compound upon irradiation with a LED at 405 nm. The photoinitiation mechanism of these photoinitiators is proposed, supported by theoretical calculations; the detection of CO2 during photopolymerization was performed by means of Fourier transform infrared spectroscopy and the detection of radical species was performed by electron spin resonance analysis. Through direct laser writing, different objects exhibiting an excellent spatial resolution could be obtained. Parallel to the photoinitiating ability, the different photoinitiators also showed a thermal initiation behavior, meaning that these structures can serve both as thermal and photo-initiators on demand. Due to the high sensitivity of these structures to sunlight, OXE-1 and OXE-5 were also investigated as solar photoinitiators (reactive also in Central Europe during winter) and excellent monomer conversions could be obtained within one hour using a multifunctional acrylate monomer (Ebecryl 605). To the best of our knowledge, these two oxime esters constitute the first examples of sunlight activable oxime esters ever reported in the literature.

利用阳光在空气中引发自由基聚合是一个关键的挑战。由于相关的低光强,通常或商业光引发剂的特点是效率低。在这项工作中,开发了17种卡唑-香豆素基肟酯,作为单组分和光裂解(I型)聚合引发剂,在可见光范围内具有优异的光吸收性能。与基准光引发剂(二苯基(2,4,6-三甲基苯甲酰)氧化膦)相比,其中一些(即OXE-1和OXE-5)在405 nm的LED照射下可以表现出与参考化合物相似或更好的光引发性能。提出了这些光引发剂的光引发机理,并进行了理论计算;采用傅里叶变换红外光谱法检测光聚合过程中的CO2,采用电子自旋共振法检测自由基种类。通过激光直接书写,可以获得具有良好空间分辨率的不同物体。除了光引发能力外,不同的光引发剂还表现出热引发行为,这意味着这些结构可以根据需要同时作为热引发剂和光引发剂。由于这些结构对阳光的高度敏感性,OXE-1和OXE-5也被研究作为太阳光引发剂(在中欧冬季也有反应),使用多功能丙烯酸酯单体(Ebecryl 605)可以在一小时内获得优异的单体转化。据我们所知,这两种肟酯构成了文献中报道的阳光活化肟酯的第一个例子。
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引用次数: 1
Vitreoscilla hemoglobin: a natural carbene transfer catalyst for diastereo- and enantioselective synthesis of nitrile-substituted cyclopropanes† 玻璃体振荡菌血红蛋白:一种天然碳转移催化剂,用于硝基取代环丙烷的非映对和对映选择性合成
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-14 DOI: 10.1039/D3GC01905E
Hanqing Xie, Fengxi Li, Yaning Xu, Chunyu Wang, Yuelin Xu, Junhao Wu, Zhengqiang Li, Zhi Wang and Lei Wang

Hemoproteins have recently emerged as attractive biocatalysts for catalyzing carbene-mediated cyclopropanation, a synthetically valuable reaction not found in nature. In this study, we present a hemoglobin-catalyzed strategy for the highly stereoselective synthesis of nitrile-substituted cyclopropanes. This method offers efficiency and environmental friendliness by utilizing an asymmetric olefin cyclopropanation reaction catalyzed by wild-type Vitreoscilla hemoglobin in the presence of in situ generated diazoacetonitrile. A diverse range of nitrile-substituted cyclopropanes could be synthesized in water with exceptional stereoselectivity, achieving up to 99.9% de and ee and high turnover numbers of up to 3232. By employing this sustainable approach, not only can various chiral nitrile-substituted cyclopropanes be efficiently obtained, but also the practical application of hemoglobin in organic synthesis can be expanded.

血红蛋白最近成为有吸引力的生物催化剂,用于催化碳介导的环丙烷化,这是一种在自然界中没有发现的有合成价值的反应。在这项研究中,我们提出了一种血红蛋白催化的高立体选择性合成腈取代环丙烷的策略。该方法利用野生型玻璃体血红蛋白在原位生成的重氮乙腈存在下催化的不对称烯烃环丙烷化反应,具有效率和环境友好性。各种腈取代的环丙烷可以在水中合成,具有优异的立体选择性,de和ee高达99.9%,周转率高达3232。采用这种可持续的方法,不仅可以高效地获得各种手性腈取代环丙烷,而且可以扩大血红蛋白在有机合成中的实际应用。
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引用次数: 2
Nano-structured hydrotrope-caged cytochrome c with boosted stability in harsh environments: a molecular insight† 纳米结构的水笼细胞色素c与提高稳定性在恶劣环境:分子的洞察力†
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-11 DOI: 10.1039/D3GC01704D
Pranav Bharadwaj, Dheeraj Kumar Sarkar, Meena Bisht, Sachin M. Shet, Nataraj Sanna Kotrappanavar, Veeresh Lokesh, Gregory Franklin, Jan Brezovsky and Dibyendu Mondal

Green and nano-structured catalytic media are vital for biocatalysis to attenuate the denaturation tendency of biocatalysts under severe reaction conditions. Hydrotropes with multi-faceted physiochemical properties represent promising systems for sustainable protein packaging. Herein, the ability of adenosine-5′-triphosphate (ATP) and cholinium salicylate ([Cho][Sal]) ionic liquid (IL) to form nano-structures and to nano-confine Cytochrome c (Cyt c) enhanced the stability and activity under multiple stresses. Experimental and computational analyses were undertaken to explain the nano-structured phenomenon of ATP and IL, structural organizations of nano-confined Cyt c, and site-specific interactions that stabilize the protein structure. Both ATP and IL form nano-structures in aqueous media and could cage Cyt c via multiple nonspecific soft interactions. Remarkably, the engineered molecular nano-cages of ATP (5–10 mM), IL (300 mg mL−1), and ATP + IL surrounding Cyt c resulted in 9-to-72-fold higher peroxidase activity than native Cyt c with exceptionally high thermal tolerance (110 °C). The polar interactions with the cardiolipin binding site of Cyt c, mediated by hydrotropes, were well correlated with the increased peroxidase activity. Furthermore, higher activity trends were observed in the presence of urea, GuHCl, and trypsin without any protein degradation. Specific binding of hydrotropes in highly mobile regions of Cyt c (Ω 40–54 residues) and enhanced H-bonding with Lys and Arg offered excellent stability under extreme conditions. Additionally, ATP effectively counteracted reactive oxygen species (ROS)-induced denaturation of Cyt c, which was enhanced by the [Sal] counterpart of IL. Overall, this study explored the robustness of nano-structured hydrotropes to have a higher potential for protein packaging with improved stability and activity under extreme conditions. Thus, the present work highlights a novel strategy for real-time industrial biocatalysis to protect mitochondrial cells from ROS-instigated apoptosis.

绿色和纳米结构的催化介质对生物催化至关重要,可以减轻生物催化剂在恶劣反应条件下的变性倾向。具有多方面理化性质的水变性物代表了可持续蛋白质包装的有前途的系统。其中,腺苷-5 ' -三磷酸腺苷(ATP)和水杨酸胆碱([Cho][Sal])离子液体(IL)形成纳米结构和纳米限制细胞色素c (Cyt c)的能力增强了在多种胁迫下的稳定性和活性。实验和计算分析解释了ATP和IL的纳米结构现象,纳米限制性Cyt c的结构组织,以及稳定蛋白质结构的位点特异性相互作用。ATP和IL在水介质中形成纳米结构,并通过多种非特异性软相互作用笼化Cyt c。值得注意的是,ATP (5-10 mM)、IL (300 mg mL - 1)和ATP + IL环绕Cyt c的纳米笼的过氧化物酶活性比天然Cyt c高9- 72倍,具有极高的耐热性(110°c)。与Cyt c的心磷脂结合位点的极性相互作用,由水异构物介导,与过氧化物酶活性的增加密切相关。此外,在尿素、GuHCl和胰蛋白酶存在的情况下,观察到更高的活性趋势,而没有任何蛋白质降解。在Cyt c的高流动区域(Ω 40-54残基)上的亲水物特异性结合以及与赖氨酸和精氨酸的h键增强,在极端条件下提供了出色的稳定性。此外,ATP有效地抵消了活性氧(ROS)诱导的Cyt c变性,而这种变性被IL的[Sal]对偶物增强。总的来说,本研究探索了纳米结构的水产物的稳健性,在极端条件下具有更高的稳定性和活性,具有更高的蛋白质包装潜力。因此,目前的工作强调了实时工业生物催化的新策略,以保护线粒体细胞免受ros诱导的凋亡。
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引用次数: 0
TXPhos: a highly stable and efficient ligand designed for ppm level Pd-catalyzed Suzuki–Miyaura coupling in water† TXPhos:一种高度稳定和高效的配体,设计用于ppm级pd催化水中的Suzuki-Miyaura偶联
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-09 DOI: 10.1039/D2GC04885J
Lei Zhang, Wenbo Hu, Heng Li, Jicheng Shi and Bingxin Yuan
An easily made and highly efficient terphenylphosphine ligand TXPhos is developed for ppm level Pd-catalyzed Suzuki-Miyaura coupling reaction in the aqueous medium. The terphenyl skeleton of TXPhos provides high stability...
开发了一种易于制备且高效的terphenylphospine配体TXPhos,用于水介质中ppm级pd催化的Suzuki-Miyaura偶联反应。TXPhos的terphenyl骨架通过增加空间体积和增强Pd -芳烃相互作用提供了高稳定性和反应性,从而导致更具催化活性的单聚Pd物种。TXPhos palladacycle在空气气氛下具有良好的产品产率,并且在胶束条件下将反应时间缩短到几分钟,TOF高达40000 s−1。
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引用次数: 0
Expanding the circularity of plastic and biochar materials by developing alternative low environmental footprint sensors 通过开发可替代的低环境足迹传感器,扩大塑料和生物炭材料的循环性
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-09 DOI: 10.1039/D3GC01103H
Rocco Cancelliere, Giuseppina Rea, Leonardo Severini, Luciana Cerri, Gabriella Leo, Elisa Paialunga, Pietro Mantegazza, Claudia Mazzuca and Laura Micheli

Flexible screen-printing technology combined with the use of a nano/material coating for improving electrode functionalities boosted the manufacturing of highly sensitive electrochemical sensors addressing the need for fast and easy-to-handle tests in different application fields. However, due to the large-scale production and disposable and single-use nature of these devices, their environmental footprint should be taken into careful consideration. Herein, the innovative reuse of post-consumer polyethene terephthalate (PET) plastics as an alternative substrate coupled with biochar as an environmentally friendly and cost-effective modifier is described as a sustainable alternative for the production of robust electrochemical sensors. The good printability of reused plastics with graphite inks despite the chemical heterogeneity, different crystallinity, and surface roughness was demonstrated using atomic force microscopy and attenuated total reflection Fourier transform infrared spectroscopy. Functionalization with brewers’ spent grain biochar enabled the fabrication of highly performing electrochemical sensors for nitrite detection in water having a limit of detection and a limit of quantification of 3.3 nM and 10.3 nM, respectively, with a linear range spanning from 0.01 to 500 μM, and good reproducibility (RSD% 8%). The innovative intervention of the biochar-multilayer system markedly enhanced the electron transfer process at the electrode interface while simultaneously serving as an absorptive material for the investigated analyte. This work lays a foundation for repurposing end-of-life plastics for the electronics industry and presents a customizable reuse strategy aimed to keep the value of plastics in the economy and reduce waste and leakage into the natural environment.

柔性丝网印刷技术结合使用纳米/材料涂层来改善电极功能,促进了高灵敏度电化学传感器的制造,满足了不同应用领域对快速和易于处理的测试的需求。然而,由于这些设备的大规模生产和一次性使用的性质,它们的环境足迹应该仔细考虑。在此,将消费后的聚对苯二甲酸乙二醇酯(PET)塑料作为替代衬底的创新再利用,加上生物炭作为环保和经济有效的改性剂,被描述为生产稳健的电化学传感器的可持续替代方案。利用原子力显微镜和衰减全反射傅里叶变换红外光谱技术证明,尽管石墨油墨的化学不均匀性、结晶度和表面粗糙度不同,但再生塑料具有良好的印刷性。利用啤酒废粮生物炭功能化制备了高性能的水中亚硝酸盐检测电化学传感器,检测限和定量限分别为3.3 nM和10.3 nM,线性范围为0.01 ~ 500 μM,重现性好(RSD% 8%)。生物炭-多层体系的创新干预显着增强了电极界面上的电子传递过程,同时作为所研究分析物的吸收材料。这项工作为电子行业重新利用报废塑料奠定了基础,并提出了一种可定制的再利用策略,旨在保持塑料在经济中的价值,减少浪费和泄漏到自然环境中。
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引用次数: 1
Improving the efficiency and sustainability of chitin bioconversion through a combination of Streptomyces chitin-active-secretomes and mechanical-milling† 通过链霉菌的几丁质活性分泌体和机械加工的结合提高几丁质生物转化的效率和可持续性
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-08 DOI: 10.1039/D3GC01084H
Lal Duhsaki, Saumashish Mukherjee and Jogi Madhuprakash

Chitin, particularly α-chitin, is the most abundant and highly recalcitrant form, fortified by an intricate network of hydrogen bonds. Efficient valorization of α-chitin requires mild pre-treatment and enzymatic hydrolysis. Streptomyces spp. secrete chitin-active CAZymes that can efficiently tackle the recalcitrant problem of chitin biomass. To better understand the potential of Streptomyces spp., a comparative analysis was performed between the novel isolate, Streptomyces sp. UH6 and the well-known chitin degraders, S. coelicolor and S. griseus. Growth studies and FE-SEM analysis revealed that all three Streptomyces spp. could utilize and degrade both α- and β-chitin. Zymogram analysis showed expression of 5–7 chitinases in the secretomes of Streptomyces strains. The chitin-active-secretomes produced by Streptomyces sp. UH6 and S. griseus were optimally active at acidic pH (pH 4.0 and 5.0) and 50 °C. Time-course degradation of α- and β-chitin with the secretomes generated N-acetyl-D-glucosamine (GlcNAc) and N,N-diacetylchitobiose [(GlcNAc)2] as the predominant products. Further, the highly crystalline α-chitin was subjected to pre-treatment by ball-milling, which reduced the crystallinity from 88% to 56.6% and increased the BET surface area by 3-folds. Of note, the activity of all three Streptomyces secretomes was improved by a mild pre-treatment, while Streptomyces sp. UH6 secretome displayed improved GlcNAc and (GlcNAc)2 yields by 14.4 and 9.6-folds, respectively. Overall, our results suggest that the Streptomyces chitin-active-secretomes, particularly Streptomyces sp. UH6, can be deployed for efficient valorization of chitin biomass and to establish an economically feasible and eco-friendly process for valorizing highly recalcitrant α-chitin.

几丁质,尤其是α-几丁质,是最丰富和最顽固的形式,由一个复杂的氢键网络加强。α-几丁质的有效活化需要温和的预处理和酶水解。链霉菌分泌的几丁质活性酶可以有效地解决几丁质生物量的顽固性问题。为了更好地了解Streptomyces spp.的潜力,我们将新分离的Streptomyces sp. UH6与著名的几质降解物S. coelicolor和S. griseus进行了比较分析。生长研究和FE-SEM分析表明,这3种链霉菌都能利用和降解α-和β-几丁质。酶谱分析显示,链霉菌分泌组中有5-7种几丁质酶的表达。Streptomyces sp. UH6和S. griseus产生的几丁质活性分泌体在酸性pH (pH 4.0和5.0)和50°C条件下具有最佳活性。分泌组降解α-和β-几丁质时,主要产物为N-乙酰-d -氨基葡萄糖(GlcNAc)和N,N-二乙酰壳聚糖[(GlcNAc)2]。对高结晶度α-几丁质进行球磨预处理,结晶度由88%降至56.6%,BET表面积增加3倍。值得注意的是,这三种链霉菌分泌组的活性都得到了温和的预处理,而链霉菌UH6分泌组的GlcNAc和(GlcNAc)2的产量分别提高了14.4倍和9.6倍。总之,我们的研究结果表明,链霉菌的几丁质活性分泌体,特别是链霉菌UH6,可以用于几丁质生物量的有效增殖,并建立一个经济上可行和环保的方法来增殖高顽固的α-几丁质。
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引用次数: 0
Selective oxidative upgrade of waste polystyrene plastics by nitric acid to produce benzoic acid† 废聚苯乙烯塑料用硝酸选择性氧化升级制苯甲酸†
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-07 DOI: 10.1039/D3GC00865G
Xi Luo, Jiahui Zhan, Qingqing Mei and Shicheng Zhang

Polystyrene plastic is a widely used artificial material, but there is still no efficient, economic or environmentally friendly recycling method for waste polystyrene plastic, which has caused serious environmental pollution and a waste of resources. Herein, the method of nitric acid oxidative upgrade is used to convert polystyrene plastic into a high-value chemical raw material, benzoic acid. The yield can reach nearly 90% at 180 °C within 3 h, and the purity of the product is more than 95%. In this process, nitric acid is decomposed by heat to generate nitrogen dioxide and oxygen, which react with the carbon-centered radicals formed at weak sites on the long chain of polystyrene and further generate peroxy radicals and hydroxyl radicals. The formation of oxygen-containing functional groups promoted the fracture of the C–C bond and eventually formed benzoic acid. In addition, this method also has good treatment effects on real-life polystyrene plastic products. This research provides a new method for the recycling and high-value utilization of waste polystyrene plastics. The intrinsic material value of polymers can be maintained by recycling functional chemicals through oxidative upgrade.

聚苯乙烯塑料是一种应用广泛的人造材料,但目前还没有一种高效、经济、环保的废旧聚苯乙烯塑料回收方法,造成了严重的环境污染和资源浪费。本文采用硝酸氧化升级法将聚苯乙烯塑料转化为高价值的化工原料苯甲酸。在180℃条件下,3 h产率可达近90%,产品纯度达95%以上。在此过程中,硝酸受热分解生成二氧化氮和氧气,二氧化氮和氧气与聚苯乙烯长链弱位点形成的碳中心自由基反应,进一步生成过氧自由基和羟基自由基。含氧官能团的形成促进了C-C键的断裂,最终形成苯甲酸。此外,该方法对现实生活中的聚苯乙烯塑料制品也有很好的处理效果。本研究为废旧聚苯乙烯塑料的回收利用和高价值利用提供了一条新途径。通过氧化升级回收功能化学品,可以保持聚合物固有的物质价值。
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引用次数: 0
Advancements and challenges in the production of low-carbon fuels via catalytic fast pyrolysis of biomass through refinery integration and co-product generation† 通过炼油厂整合和副产品生成生物质催化快速热解生产低碳燃料的进展和挑战
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2023-08-07 DOI: 10.1039/D3GC01574B
Matthew M. Yung, Calvin Mukarakate, Kristiina Iisa, A. Nolan Wilson, Mark R. Nimlos, Susan E. Habas, Abhijit Dutta, Kinga A. Unocic, Joshua A. Schaidle and Michael B. Griffin

The production of advanced biofuels represents a near-term opportunity to decarbonize the heavy vehicle transportation sector. However, important barriers must be overcome and successful deployment of these technologies will require (i) catalyst and process development to reduce cost and improve carbon utilization and (ii) industry-relevant validation of operability to de-risk scale-up. Herein, we seek to address these challenges for an integrated two-step process involving catalytic fast pyrolysis (CFP) followed by co-hydrotreating of bio-oil with refinery streams. Technoeconomic and lifecycle analysis based on the data presented herein reveal the potential to generate low-carbon transportation fuels and chemical co-products with a modelled selling price of $2.83 gasoline gallon equivalent (2016$) and a 78% reduction in greenhouse gas emissions compared to fossil-based pathways. The feedstock for this research was a blend of 50 wt% loblolly pine and 50 wt% waste forest residues, and the CFP step was performed using an ex situ fixed bed of Pt/TiO2 with co-fed H2 at atmospheric pressure. Compared to previous state-of-technology benchmarks, advancements in catalyst design and synthesis methodology enabled a four-fold reduction in Pt loading and a 400% increase in time on stream without negatively impacting upgrading performance. Additionally, a first-of-its-kind integrated assessment of waste gas adsorption showed near quantitative recovery of acetone and 2-butanone, which collectively represent approximately 5% of the biomass carbon. The valorization of these co-products opens opportunities to support decarbonization of the chemical sector while simultaneously improving the overall process carbon efficiency to >40%. After condensation, the CFP-oil was co-hydrotreated with straight run diesel (10 : 90 vol%) to achieve 95% biogenic carbon incorporation. The oxygen content of the hydrotreated oil was below detection limits, and the diesel fraction exhibited a cetane number and cloud point suitable for a finished fuel. This manuscript concludes by highlighting remaining research needs associated with improving thermal management during catalyst regeneration, mitigating catalyst deactivation due to inorganic deposition, and demonstrating the durability of biomass feeding systems when operated in hydrogen-rich environments.

先进生物燃料的生产代表了重型车辆运输部门脱碳的近期机会。然而,必须克服重要的障碍,这些技术的成功部署将需要(i)催化剂和工艺开发,以降低成本和提高碳利用率;(ii)与行业相关的可操作性验证,以减少风险的扩大。在此,我们寻求解决这些挑战的集成两步工艺,包括催化快速热解(CFP),然后与炼油厂流共加氢处理生物油。基于本文提供的数据的技术经济和生命周期分析表明,与化石燃料相比,低碳运输燃料和化学副产品的模型售价为2.83美元汽油加仑当量(2016年美元),温室气体排放量减少78%。本研究的原料是50%火炬松和50%森林废弃物的混合物,CFP步骤是在常压下使用Pt/TiO2的非原位固定床和共进料H2进行的。与之前的技术基准相比,催化剂设计和合成方法的进步使Pt负载减少了4倍,生产时间增加了400%,而不会对升级性能产生负面影响。此外,对废气吸附的首次综合评估显示,丙酮和2-丁酮的回收率接近定量,它们总共约占生物质碳的5%。这些副产品的增值为支持化工行业的脱碳提供了机会,同时将整个过程的碳效率提高到40%。冷凝后,cfp油与直馏柴油(10:90 vol%)共加氢处理,达到95%的生物炭掺入率。加氢处理后的油氧含量低于检测限值,柴油馏分呈现出适合成品燃料的十六烷值和浊点。本文最后强调了与改善催化剂再生过程中的热管理、减轻无机沉积引起的催化剂失活以及在富氢环境中运行时生物质投料系统的耐久性相关的剩余研究需求。
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引用次数: 0
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