biorefinery

生物炼制
  • 文章类型: Journal Article
    双组分系统(TCS)是细菌中普遍存在的信号通路。这些系统介导组氨酸激酶和反应调节剂之间的磷酸转移,促进对不同身体的反应,化学,和生物刺激。合成和结构生物学的进步使TCS重新用于监测重金属,疾病相关生物标志物,和生物产品的生产。然而,由于缺乏有效的工程方法,许多TCS生物传感器的实用性受到不良性能的阻碍。这里,我们简要讨论了TCS的架构和监管机制。我们还总结了TCS工程的最新进展,通过实验或基于计算的方法来微调生物传感器的功能参数,如反应曲线和特异性。工程TCS在医疗领域具有巨大的潜力,环境,和生物炼制领域,在广泛的生物技术领域发挥着关键作用。
    Two-component systems (TCSs) are prevalent signaling pathways in bacteria. These systems mediate phosphotransfer between histidine kinase and a response regulator, facilitating responses to diverse physical, chemical, and biological stimuli. Advancements in synthetic and structural biology have repurposed TCSs for applications in monitoring heavy metals, disease-associated biomarkers, and the production of bioproducts. However, the utility of many TCS biosensors is hindered by undesired performance due to the lack of effective engineering methods. Here, we briefly discuss the architecture and regulatory mechanisms of TCSs. We also summarize the recent advancements in TCS engineering by experimental or computational-based methods to fine-tune the biosensor functional parameters, such as response curve and specificity. Engineered TCSs have great potential in the medical, environmental, and biorefinery fields, demonstrating a crucial role in a wide area of biotechnology.
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  • 文章类型: Journal Article
    通过利用羟基自由基作为化学引发剂,超声波辐射具有选择性氧化水相中非挥发性有机底物的潜力。这里,通过从光解和辐射化学中收集见解来构建羟基自由基引发的乙二醛氧化的机理描述,以解释氧化产物的产率和动力学趋势。本文报道的机理描述和动力学测量表明,与来自C-C裂解的那些产物相比,通过改变超声频率增加羟基自由基的形成速率增加乙二醛消耗速率和对C2酸产物的选择性两者。在酸性条件下,乙二醛的消耗也发生得更快,对C2酸的选择性更高。这有利于羧酸酯中间体质子化为其反应性较低的酸性形式。利用这样的pH和频率效应对于通过与羟基自由基和氧化产物(特别是过氧化氢和超氧化物)的副反应来减轻产物降解是至关重要的。这些发现证明了超声作为醛官能团选择性氧化为羧酸的驱动器的潜力,为生物质衍生的平台分子提供了一条可持续的途径。
    Ultrasonic irradiation holds potential for the selective oxidation of non-volatile organic substrates in the aqueous phase by harnessing hydroxyl radicals as chemical initiators. Here, a mechanistic description of hydroxyl radical-initiated glyoxal oxidation is constructed by gleaning insights from photolysis and radiation chemistry to explain the yields and kinetic trends for oxidation products. The mechanistic description and kinetic measurements reported herein reveal that increasing the formation rate of hydroxyl radicals by changing the ultrasound frequency increases both the rates of glyoxal consumption and the selectivity towards C2 acid products over those from C-C cleavage. Glyoxal consumption also occurs more rapidly and with greater selectivity towards C2 acids under acidic conditions, which favor the protonation of carboxylate intermediates into their less reactive acidic forms. Leveraging such pH and frequency effects is crucial to mitigating product degradation by secondary reactions with hydroxyl radicals and oxidation products (specifically hydrogen peroxide and superoxide). These findings demonstrate the potential of ultrasound as a driver for the selective oxidation of aldehyde functions to carboxylic acids, offering a sustainable route for valorizing biomass-derived platform molecules.
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  • 文章类型: Journal Article
    开发了一种由氯化胆碱(ChCl)基低共熔溶剂(DES)和甲基异丁基酮(MIBK)组成的简便两相体系,以实现糠醛的生产。一锅法从桉树中分离木质素并制备可发酵葡萄糖。结果表明,ChCl/1,2-丙二醇/MIBK体系具有将半纤维素转化为糠醛的最佳性能。在最佳条件下(MRChCl:1,2-丙二醇=1:2,原料:DES:MIBK比例=1:4:8g/g/mL,0.075mol/LAlCl3·6H2O,140°C,和90分钟),糠醛产率和葡萄糖产率分别达到65.0和92.2%,分别。同时,低分子量木质素(1250-1930g/mol),低多分散性(DM=1.25-1.53)和高纯度(碳水化合物含量仅为0.08-2.59%)从两相系统中再生。随着预处理温度的升高,再生木质素中的β-O-4、β-β和β-5键逐渐断裂,酚羟基的含量增加,但脂肪族羟基的含量下降。该研究为生物炼制过程中木质纤维素的综合利用提供了新的策略。
    A facile biphasic system composed of choline chloride (ChCl)-based deep eutectic solvent (DES) and methyl isobutyl ketone (MIBK) was developed to realize the furfural production, lignin separation and preparation of fermentable glucose from Eucalyptus in one-pot. Results showed that the ChCl/1,2-propanediol/MIBK system owned the best property to convert hemicelluloses into furfural. Under the optimal conditions (MRChCl:1,2-propanediol = 1:2, raw materials:DES:MIBK ratio = 1:4:8 g/g/mL, 0.075 mol/L AlCl3·6H2O, 140 °C, and 90 min), the furfural yield and glucose yield reached 65.0 and 92.2 %, respectively. Meanwhile, the lignin with low molecular weight (1250-1930 g/mol), low polydispersity (DM = 1.25-1.53) and high purity (only 0.08-2.59 % carbohydrate content) was regenerated from the biphasic system. With the increase of pretreatment temperature, the β-O-4, β-β and β-5 linkages in the regenerated lignin were gradually broken, and the content of phenolic hydroxyl groups increased, but the content of aliphatic hydroxyl groups decreased. This research provides a new strategy for the comprehensive utilization of lignocellulose in biorefinery process.
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  • 文章类型: Journal Article
    木质纤维素的水解和生物转化,即,生物炼制,可以为人类提供生物燃料,生物基化学品,和材料,是解决化石能源危机、促进全球可持续发展的重要技术。生物炼制包括预处理等步骤,糖化,和发酵,近年来,研究人员开发了多种生物精炼策略来优化工艺并降低工艺成本。木质纤维素水解产物是连接糖化过程和下游发酵的平台。水解物组成与生物质原料密切相关,预处理过程,以及生物精炼策略的选择,不仅为下游发酵提供营养,还提供可能的抑制剂。在这次审查中,我们总结了木质纤维素生物炼制各阶段对营养物质和可能的抑制剂的影响,分析了各种生物炼制策略在营养保留和抑制剂产生方面的巨大差异,并强调木质纤维素生物炼制的所有步骤都需要综合考虑,以低成本实现最大限度的营养保留和抑制剂的最佳控制,为生物质能源和化工的发展提供参考。
    The hydrolysis and biotransformation of lignocellulose, i.e., biorefinery, can provide human beings with biofuels, bio-based chemicals, and materials, and is an important technology to solve the fossil energy crisis and promote global sustainable development. Biorefinery involves steps such as pretreatment, saccharification, and fermentation, and researchers have developed a variety of biorefinery strategies to optimize the process and reduce process costs in recent years. Lignocellulosic hydrolysates are platforms that connect the saccharification process and downstream fermentation. The hydrolysate composition is closely related to biomass raw materials, the pretreatment process, and the choice of biorefining strategies, and provides not only nutrients but also possible inhibitors for downstream fermentation. In this review, we summarized the effects of each stage of lignocellulosic biorefinery on nutrients and possible inhibitors, analyzed the huge differences in nutrient retention and inhibitor generation among various biorefinery strategies, and emphasized that all steps in lignocellulose biorefinery need to be considered comprehensively to achieve maximum nutrient retention and optimal control of inhibitors at low cost, to provide a reference for the development of biomass energy and chemicals.
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  • 文章类型: Journal Article
    木质纤维素生物炼制依赖于有效的预处理策略对于解决当前全球生态系统和能源安全危机具有重要意义。本研究提出了一种结合海水水热预处理(SHP)和微波辅助深度共晶溶剂(MD)预处理的新方法,以实现马尾松有效分馏为高附加值产品。结果表明,复合离子(Mg2+,Ca2+,和Cl-)在天然海水中充当路易斯酸,并显着促进甘露糖和木聚糖解聚为寡糖,产率为40.17%和75.43%,分别。随后的MD处理实现了快速有效的木质素分馏(~90%),同时保留了纤维素。因此,综合预处理产生约85%的酶促葡萄糖,表明与未经处理的松树相比增加了八倍。由于在MD处理期间由酰基的形成引起的疏水性增加,从DES中成功地回收了均匀的木质素纳米球。它表现出低分散性(PDI=2.23),小分子量(1889克/摩尔),和优异的抗氧化性(RSI=5.94),在功能材料中展示了有希望的应用。通过FTIR对木质素解聚机理进行了全面的阐明,2D-HSQCNMR,和GPC分析。总的来说,本研究为木质纤维素生物炼制和木质素增值提供了一种新的环保策略。
    Lignocellulose biorefinery depended on effective pretreatment strategies is of great significance for solving the current global crisis of ecosystem and energy security. This study proposes a novel approach combining seawater hydrothermal pretreatment (SHP) and microwave-assisted deep eutectic solvent (MD) pretreatment to achieve an effective fractionation of Pinus massoniana into high value-added products. The results indicated that complex ions (Mg2+, Ca2+, and Cl-) in natural seawater served as Lewis acids and dramatically promoted the depolymerization of mannose and xylan into oligosaccharides with 40.17 % and 75.43 % yields, respectively. Subsequent MD treatment realized a rapid and effective lignin fractionation (~90 %) while retaining cellulose. As a result, the integrated pretreatment yielded ~85 % of enzymatic glucose, indicating an eightfold increase compared with untreated pine. Because of the increased hydrophobicity induced by the formation of acyl groups during MD treatment, uniform lignin nanospheres were successfully recovered from the DES. It exhibited low dispersibility (PDI = 2.23), small molecular weight (1889 g/mol), and excellent oxidation resistance (RSI = 5.94), demonstrating promising applications in functional materials. The mechanism of lignin depolymerization was comprehensively elucidated via FTIR, 2D-HSQC NMR, and GPC analyses. Overall, this study provides a novel and environmentally friendly strategy for lignocellulose biorefinery and lignin valorization.
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  • 文章类型: Journal Article
    微生物将农业食品废物转化为有价值的化合物提供了发展生物经济的可持续途径,并有助于可持续的生物炼制。酪丁酸梭菌表现出一系列适用于农业食品垃圾高产转化的天然性状,这使得它成为生产各种化合物的有前途的宿主,如短链脂肪酸及其衍生酯产品。在这项研究中,在酪丁酸梭菌中构建了丁醇合成途径,然后通过向发酵中添加脂肪酶,通过原位酯化实现高效生产丁酸丁酯。丁酰-CoA/酰基-CoA转移酶(cat1)被过表达以平衡前体丁酸和丁醇之间的比例。然后,以木糖为唯一碳源,虾壳废物为唯一氮源,获得了适合丁酸丁酯生产的发酵培养基。最终,5.9g/L的丁酸丁酯,选择性为100%,在5L生物反应器中分批发酵的木糖和虾壳废物下,生产率达到0.03g/L·h。转录组分析显示与木糖代谢相关的基因表达增加,氮代谢,氨基酸代谢和运输,揭示了木糖与虾壳废弃物协同利用的机理。本研究提出了一种利用木糖和虾壳废物生产丁酸丁酯的新方法,方法是使用基于酪丁酸梭菌的厌氧发酵平台。这种创新的发酵培养基可以节省氮源的成本(约97%),并为将农业食品垃圾转化为其他高价值产品开辟了可能性。
    Microbial conversion of agri-food waste to valuable compounds offers a sustainable route to develop the bioeconomy and contribute to sustainable biorefinery. Clostridium tyrobutyricum displays a series of native traits suitable for high productivity conversion of agri-food waste, which make it a promising host for the production of various compounds, such as the short-chain fatty acids and their derivative esters products. In this study, a butanol synthetic pathway was constructed in C. tyrobutyricum, and then efficient butyl butyrate production through in situ esterification was achieved by the supplementation of lipase into the fermentation. The butyryl-CoA/acyl-CoA transferase (cat1) was overexpressed to balance the ratio between precursors butyrate and butanol. Then, a suitable fermentation medium for butyl butyrate production was obtained with xylose as the sole carbon source and shrimp shell waste as the sole nitrogen source. Ultimately, 5.9 g/L of butyl butyrate with a selectivity of 100%, and a productivity of 0.03 g/L·h was achieved under xylose and shrimp shell waste with batch fermentation in a 5 L bioreactor. Transcriptome analyses exhibited an increase in the expression of genes related to the xylose metabolism, nitrogen metabolism, and amino acid metabolism and transport, which reveal the mechanism for the synergistic utilization of xylose and shrimp shell waste. This study presents a novel approach for utilizing xylose and shrimp shell waste to produce butyl butyrate by using an anaerobic fermentative platform based on C. tyrobutyricum. This innovative fermentation medium could save the cost of nitrogen sources (~97%) and open up possibilities for converting agri-food waste into other high-value products.
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  • 文章类型: Journal Article
    将木质素转化为芳香化学品是一种高价值利用木质纤维素原料的有前途的策略。然而,木质素的固有异质性对在生物精炼系统中实现有效转化和最佳产品产量构成了重大障碍。在这里,我们采用一步分级分离方法来增强木质素的均匀性,并利用THF/DMSO-EtONa(四氢呋喃/二甲基亚砜-乙醇钠)系统来解聚分馏的木质素。使用三种质子溶剂和三种非质子溶剂进行分馏。研究了溶剂性质对分馏木质素的结构和解聚效率的影响。甲醇分馏木质素产生的苯甲酸化合物的产率为30重量%,比未分馏的木质素高50%。极性(δP),氢键能力(δH),选择的质子溶剂的粘度(η)与分子量(Mw)表现出强的线性相关,聚合物分散指数(PDI),和分级分离的木质素的丁香基/愈创酰基比(S/G比),以及由β-O-4键断裂衍生的苯甲酸化合物的总产率。这项研究阐明了溶剂性质与木质素结构之间的关系,并提出了一种有希望的方法来精炼木质素以提高利用效率,从而提出了复杂木质素聚合物增值应用的潜在策略。
    Converting lignin into aromatic chemicals is a promising strategy for the high-value utilization of lignocellulosic feedstock. However, the inherent heterogeneity of lignin poses a significant obstacle to achieving efficient conversion and optimal product yields within bio-refinery systems. Herein, we employed a one-step fractionation method to enhance lignin homogeneity and utilized the THF/DMSO-EtONa (tetrahydrofuran/dimethyl sulfoxide-sodium ethoxide) system to depolymerize the fractionated lignin. Three protic and three aprotic solvents were used for fractionation. The impact of the solvent properties on the structure and the depolymerization efficiency of the fractionated lignin was investigated. Methanol-fractionated lignin generated the benzoic acid compounds with a yield of 30 wt%, 50 % higher than that of the unfractionated lignin. The polarities (δP), hydrogen bonding abilities (δH), and viscosities (η) of selected protic solvents showed strong linear correlation with molecular weight (Mw), polymer dispersity index (PDI), and syringyl/guaiacyl ratio (S/G ratio) of the fractionated lignin, as well as the total yield of benzoic acid compounds derived from the β-O-4 bond cleavage. This study elucidates the relationship between solvent properties and lignin structure and proposes a promising approach for refining lignin to enhance utilization efficiency, thereby presenting a potential strategy for value-added application of complex lignin polymers.
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  • 文章类型: Journal Article
    这里,白酒酒糟(BDG)用于生物炼制开发,以产生增值的副产物和生物乙醇。通过乙酸乙酯以1:6的固液比萃取10小时,取得了重大成果,包括100%的乳酸和92%的酚类回收率。剩余的BDG还实现了99%的葡聚糖回收和81%的葡聚糖至葡萄糖转化。剩余BDG在30%载量下的同时糖化和发酵产生78.5g生物乙醇/L,产率为94%。生物乙醇的最低售价从0.149-0.836美元/公斤不等,视联产品市场价格而定。与传统生产88千克玉米乳酸相比,一吨BDGs的生物炼制加工导致温室气体排放量减少了60%,70公斤抗氧化剂酚类,234公斤大豆蛋白,和225公斤玉米生物乙醇,以及BDG垃圾填埋场的排放。生物精炼厂证明了具有成本效益的生物乙醇生产和低碳排放BDG处理的协同模型。
    Here, Baijiu distillers\' grains (BDGs) were employed in biorefinery development to generate value-added co-products and bioethanol. Through ethyl acetate extraction at a 1:6 solid-liquid ratio for 10 h, significant results were achieved, including 100 % lactic acid and 92 % phenolics recovery. The remaining BDGs also achieved 99 % glucan recovery and 81 % glucan-to-glucose conversion. Simultaneous saccharification and fermentation of remaining BDGs at 30 % loading resulted in 78.5 g bioethanol/L with a yield of 94 %. The minimum selling price of bioethanol varies from $0.149-$0.836/kg, contingent on the co-product market prices. The biorefinery processing of one ton of BDGs caused a 60 % reduction in greenhouse gas emissions compared to that of the traditional production of 88 kg corn-lactic acid, 70 kg antioxidant phenolics, 234 kg soybean protein, and 225 kg corn-bioethanol, along with emissions from BDG landfilling. The biorefinery demonstrated a synergistic model of cost-effective bioethanol production and low-carbon emission BDGs treatment.
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  • 文章类型: Journal Article
    生物表面活性剂由于其性质优于化石衍生的对应物而最近引起了越来越多的关注。虽然生产成本仍然是超过合成表面活性剂的重要障碍,预计生物表面活性剂将在未来几十年获得更大的市场份额。其中,糖脂,一种低分子量的生物表面活性剂,因其降低表面和界面张力的功效而脱颖而出,这使得它们在各种表面活性剂相关的应用中备受追捧。糖脂由通过酯键与疏水性脂肪酸链连接的亲水性碳水化合物部分组成,主要包括鼠李糖脂。海藻糖脂质,槐糖脂,和甘露糖赤藓糖醇脂质。这篇综述突出了糖脂的现状,涵盖了特定的糖脂生产率和全球市场上发现的各种产品。应用,如生物修复,食品加工,石油精炼,生物医学用途,并讨论了增加农业产出的问题。此外,还彻底研究了糖脂生产成本降低的最新进展以及利用第二代原料进行可持续生产的挑战。总的来说,这项审查建议在环境优势之间取得平衡,经济可行性,通过在生物表面活性剂生产中优化二次原料的整合和社会效益。
    Biosurfactants have garnered increased attention lately due to their superiority of their properties over fossil-derived counterparts. While the cost of production remains a significant hurdle to surpass synthetic surfactants, biosurfactants have been anticipated to gain a larger market share in the coming decades. Among these, glycolipids, a type of low-molecular-weight biosurfactant, stand out for their efficacy in reducing surface and interfacial tension, which made them highly sought-after for various surfactant-related applications. Glycolipids are composed of hydrophilic carbohydrate moieties linked to hydrophobic fatty acid chains through ester bonds that mainly include rhamnolipids, trehalose lipids, sophorolipids, and mannosylerythritol lipids. This review highlights the current landscape of glycolipids and covers specific glycolipid productivity and the diverse range of products found in the global market. Applications such as bioremediation, food processing, petroleum refining, biomedical uses, and increasing agriculture output have been discussed. Additionally, the latest advancements in production cost reduction for glycolipid and the challenges of utilizing second-generation feedstocks for sustainable production are also thoroughly examined. Overall, this review proposes a balance between environmental advantages, economic viability, and societal benefits through the optimized integration of secondary feedstocks in biosurfactant production.
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  • 文章类型: Journal Article
    木质素,地球上最普遍的天然多酚来源,为转化为芳族化合物提供了大量的可能性,这对于实现可持续性和碳中和至关重要。氢转移方法由于其环境相容性和经济可行性而引起了极大的兴趣。这种方法的效力取决于催化和供氢系统的仔细选择,所述催化和供氢系统决定性地影响由木质素降解产生的单体产物的产率和选择性。本文重点介绍了木质素炼油厂的氢转移技术,特别关注氢供体对木质素解聚途径的影响。它描述了催化氢转移排列的结构和活性与木质素衍生的生化物质的色域之间的相关性,利用木质素模型化合物的数据,分离的木质素,和木质纤维素生物质。此外,本文探讨了采用氢转移方法进行木质素转化的优势和未来方向。实质上,这一概念研究阐明了氢转移范式在木质素增值中的功效,提供关键见解和战略指令,以可持续地最大化木质素的价值。
    Lignin, the most prevalent natural source of polyphenols on Earth, offers substantial possibilities for the conversion into aromatic compounds, which is critical for attaining sustainability and carbon neutrality. The hydrogen-transfer method has garnered significant interest owing to its environmental compatibility and economic viability. The efficacy of this approach is contingent upon the careful selection of catalytic and hydrogen-donating systems that decisively affect the yield and selectivity of the monomeric products resulting from lignin degradation. This paper highlights the hydrogen-transfer technique in lignin refinery, with a specific focus on the influence of hydrogen donors on the depolymerization pathways of lignin. It delineates the correlation between the structure and activity of catalytic hydrogen-transfer arrangements and the gamut of lignin-derived biochemicals, utilizing data from lignin model compounds, separated lignin, and lignocellulosic biomass. Additionally, the paper delves into the advantages and future directions of employing the hydrogen-transfer approach for lignin conversion. In essence, this concept investigation illuminates the efficacy of the hydrogen-transfer paradigm in lignin valorization, offering key insights and strategic directives to maximize lignin\'s value sustainably.
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