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Role of advanced oxidation processes in lignocellulose pretreatment towards biorefinery applications: a review on emerging trends and economic considerations 高级氧化工艺在木质纤维素预处理中对生物精炼应用的作用:新趋势和经济考虑因素综述
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-12 DOI: 10.1039/d3gc05108k
Alessia Di Fraia, Simona Di Fraia, Godvin Sharmila V, Rajesh Banu J, Nicola Massarotti
Renewable energy sources have been recognized as a viable alternative to fossil fuels. Among them, lignocellulosic biomass has emerged as a promising option for producing valuable bio-products, especially employing residual or waste material due to its consistency, reliability, local availability, and carbon neutrality. However, its efficient utilization is limited by the recalcitrance of cell walls, mainly caused by two chemical compounds, hemicellulose and lignin, reducing the accessibility to cellulose. Consequently, the hemicellulose and/or lignin in the cell wall need to be removed or rearranged to increase the accessibility to cellulose through the pretreatment of lignocellulosic biomass. Among the different pretreatments, oxidative processes efficiently enhance the digestibility of cellulose in lignocellulosic biomass, breaking down the complex structure of lignocellulosic biomass and making it more accessible for subsequent enzymatic or microbial degradation. Moreover, oxidative processes improve the reaction kinetics, are versatile in treating a wide range of lignocellulosic feedstocks, and reduce the generation of waste products. Therefore, this review aims to provide a detailed overview of the properties and composition of lignocellulosic biomass, its potential, and a comprehensive analysis of oxidative pretreatments, their advancements and recently developed innovative technologies. Furthermore, the application and economic feasibility of utilizing lignocellulosic biomass and the key obstacles hindering its widespread adoption are highlighted in this review.
可再生能源已被视为化石燃料的可行替代品。其中,木质纤维素生物质因其一致性、可靠性、本地可用性和碳中和性,已成为生产有价值生物产品的一种有前途的选择,特别是利用残余或废料。然而,由于细胞壁的不稳定性(主要是由半纤维素和木质素这两种化合物造成的),降低了纤维素的可获取性,从而限制了其有效利用。因此,需要通过对木质纤维素生物质进行预处理,去除或重新排列细胞壁中的半纤维素和/或木质素,以提高纤维素的可及性。在不同的预处理方法中,氧化工艺可有效提高木质纤维素生物质中纤维素的消化率,分解木质纤维素生物质的复杂结构,使其更容易被后续的酶或微生物降解。此外,氧化工艺还能改善反应动力学,在处理各种木质纤维素原料时用途广泛,并能减少废品的产生。因此,本综述旨在详细概述木质纤维素生物质的特性和组成、其潜力,并全面分析氧化预处理方法、其进展和最新开发的创新技术。此外,本综述还强调了利用木质纤维素生物质的应用和经济可行性,以及阻碍其广泛应用的主要障碍。
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引用次数: 0
Key challenges and advancements toward fast-charging all-solid-state lithium batteries 实现全固态锂电池快速充电的主要挑战和进展
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4gc01068j
Niaz Ahmad, Cailing Fan, Muhammad Faheem, Xiaoxiao Liang, Yirong Xiao, Xinting Cao, Chaoyuan Zeng, Qinxi Dong, Wen Yang
Next-generation energy storage systems rely heavily on the capability of fast charging as they allow electronic devices to be charged within a remarkably brief period. The practical applications of fast-charging technology are severely hindered by unsatisfactory electrochemical performance, e.g., low specific capacity, low areal capacity, low coulombic efficiency, and very limited life span, resulting in a fast-discharging process. This comprehensive review provides a concise overview of the obstacles faced and thereby the recent advancements made in the realm of fast-charging all-solid-state lithium batteries. Firstly, it explains the inherent challenges of solid-state electrolytes (SSEs) and conventional ASSLB design that impede fast-charging capabilities. Based on these challenges, the specifications and strategies for optimizing the SSEs, electrodes, and electrode/SSE interfaces are discussed to achieve the fast-charging phenomenon in ASSLBs. To give readers a better understanding of ASSLBs under fast-charging capabilities, a comprehensive conclusion and novel points of view are included in the prospects.
下一代储能系统在很大程度上依赖于快速充电能力,因为它们可以在极短的时间内为电子设备充电。快速充电技术的实际应用受到电化学性能不尽如人意的严重阻碍,例如比容量低、面积容量低、库仑效率低以及寿命非常有限,从而导致快速放电过程。本综述简明扼要地概述了快速充电全固态锂电池领域所面临的障碍,以及最近取得的进展。首先,它解释了固态电解质(SSE)和传统全固态锂电池设计所面临的固有挑战,这些挑战阻碍了快速充电能力。根据这些挑战,讨论了优化固态电解质、电极和电极/固态电解质界面的规格和策略,以实现全固态锂电池的快速充电现象。为了让读者更好地理解快速充电功能下的 ASSLB,本研究还在展望中给出了全面的结论和新颖的观点。
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引用次数: 0
Improved separation of rare earth elements using hydrophobic deep eutectic solvents: liquid–liquid extraction to selective dissolution 利用疏水性深共晶溶剂改进稀土元素的分离:从液液萃取到选择性溶解
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-11 DOI: 10.1039/d4gc01089b
Takafumi Hanada, Nicolas Schaeffer, Masahiro Katoh, Joao A. P. Coutinho, Masahiro Goto
Deep eutectic solvents (DESs) composed of a beta-diketone and phosphine oxides featuring different alkyl chain lengths were prepared and then employed as liquid–liquid extraction and dissolution media for the separation of iron, cobalt, neodymium, and dysprosium. In the dissolution the more sterically hindered DESs exhibited enhanced selectivity to neodymium, which was poorly separated using liquid–liquid extraction. The dissolution selectivity in less sterically hindered DESs could be controlled by the addition of organic acids with different alkyl chain lengths.
制备了由β-二酮和具有不同烷基链长的膦氧化物组成的深共晶溶剂(DES),并将其用作液-液萃取和溶解介质,用于分离铁、钴、钕和镝。在溶解过程中,立体受阻程度较高的 DES 对钕的选择性增强,而使用液液萃取法分离钕的效果较差。立体阻碍较小的 DES 的溶解选择性可通过添加不同烷基链长的有机酸来控制。
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引用次数: 0
Correction: Sustainable electrochemical synthesis of dry formaldehyde from anhydrous methanol 更正:从无水甲醇中可持续地电化学合成干甲醛
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-10 DOI: 10.1039/d4gc90078b
Florian Schwarz, Elizabeth Larenz, Anna K. Mechler
Correction for ‘Sustainable electrochemical synthesis of dry formaldehyde from anhydrous methanol’ by Florian Schwarz et al., Green Chem., 2024, 26, 4645–4652, https://doi.org/10.1039/D3GC04978G.
Florian Schwarz 等人撰写的 "从无水甲醇中可持续电化学合成干甲醛 "的更正,《绿色化学》,2024 年,26 期,4645-4652,https://doi.org/10.1039/D3GC04978G。
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引用次数: 0
Rational bottom-up synthesis of sulphur-rich porous carbons for single-atomic platinum catalyst supports 自下而上合理合成用于单原子铂催化剂载体的富硫多孔碳
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-09 DOI: 10.1039/d4gc02055c
Koki Chida, Takeharu Yoshii, Ryo Kawaguchi, Masataka Inoue, Fumito Tani, Tatsuki Sobue, Shunsuke Ohtani, Kenichi Kato, Tomoki Ogoshi, Shoko Nakahata, Kazuhide Kamiya, Hirotomo Nishihara
Single-atomic metal catalysts are attractive for green chemistry in terms of their outstanding catalytic performance and savings in precious metal usage owing to maximized metal utilization, including anode catalysts in polymer electrolyte fuel cells (PEFCs). Heteroatom-doped porous carbons are extensively used as supports, where the heteroatoms contribute to the immobilization of single-atomic metals. However, high-content doping of heteroatoms, especially sulphur (S), into carbon supports is still challenging because S species can be readily desorbed during heat treatment. Herein, we present a bottom-up fabrication approach for S-rich porous carbons from molecular precursors via a thermal polymerization process. A simple carbonization of molecules with thermally stable S-containing building blocks and polymerizable ethynyl moieties at 900 °C yields microporous carbon materials with record-high S content (over 15 wt%). The abundant S species function as an effective anchoring site for single-atomic platinum (Pt) species. Toward anode catalysts in PEFCs, the prepared single-atomic Pt catalysts efficiently promote the electrochemical hydrogen oxidation reaction, whose activity is comparable to that of commercial Pt/C, despite the significantly low Pt loading amount.
单原子金属催化剂具有出色的催化性能,并能最大限度地利用金属,从而节省贵金属用量,因此对绿色化学(包括聚合物电解质燃料电池(PEFC)中的阳极催化剂)很有吸引力。掺杂杂原子的多孔碳被广泛用作载体,其中的杂原子有助于固定单原子金属。然而,将杂质原子(尤其是硫(S))高含量掺杂到碳支撑物中仍然具有挑战性,因为 S 物种在热处理过程中很容易被解吸。在此,我们提出了一种自下而上的方法,通过热聚合工艺,利用分子前驱体制造富含 S 的多孔碳。在 900 °C 的温度下,对具有热稳定含 S 构建块和可聚合乙炔基的分子进行简单的碳化处理,就能得到 S 含量创纪录地高(超过 15 wt%)的微孔碳材料。丰富的 S 物质可作为单原子铂 (Pt) 物质的有效锚定位点。作为 PEFCs 的阳极催化剂,所制备的单原子铂催化剂能有效促进电化学氢氧化反应,尽管铂负载量很低,但其活性与商用 Pt/C 相当。
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引用次数: 0
Balancing computational chemistry's potential with its environmental impact 平衡计算化学的潜力和对环境的影响
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-08 DOI: 10.1039/d4gc01745e
Oliver Schilter, Philippe Schwaller, Teodoro Laino
Computational chemistry techniques offer tremendous potential for accelerating the discovery of sustainable chemical processes and reactions. However, the environmental impacts of the substantial computing power required for these digital methods are often overlooked. This review provides a comprehensive analysis of the carbon footprint associated with molecular simulations, machine learning, optimization algorithms, and the required data center and research activities within the field of digital chemistry. Successful applications of these methods tackling climate-related issues like CO2 conversion and storage are highlighted, contrasted with assessments of their environmental burden. Strategies to minimize the carbon emissions from computational efforts are evaluated, including sustainable data center practices, efficient coding, reaction optimization, and sustainable research culture. Additionally, we surveyed tools and methodologies for tracking and reporting environmental impacts. Overall, guidelines and best practices are distilled for balancing the green potential of computational chemistry with responsible management of its environmental costs. Assessing and mitigating the field's carbon footprint is crucial for ensuring digital chemical discoveries truly contribute to sustainability goals.
计算化学技术为加速发现可持续的化学过程和反应提供了巨大的潜力。然而,这些数字方法所需的大量计算能力对环境的影响往往被忽视。本综述全面分析了与分子模拟、机器学习、优化算法以及数字化学领域所需的数据中心和研究活动相关的碳足迹。重点介绍了这些方法在解决二氧化碳转化和封存等气候相关问题方面的成功应用,并对其环境负担进行了评估。我们评估了最大限度减少计算工作碳排放的策略,包括可持续数据中心实践、高效编码、反应优化和可持续研究文化。此外,我们还调查了跟踪和报告环境影响的工具和方法。总之,我们提炼出了指导方针和最佳实践,以平衡计算化学的绿色潜力和对其环境成本的负责任管理。评估和减少该领域的碳足迹对于确保数字化学发现真正有助于实现可持续发展目标至关重要。
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引用次数: 0
Correction: Metal-free visible-light-induced phosphorylation of unactivated alkyl iodides with white phosphorus as the P-atom source 更正:以白磷为 P 原子源,无金属可见光诱导未活化烷基碘化物的磷酸化反应
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-05 DOI: 10.1039/d4gc90072c
Fushan Chen, Jialiang Peng, Yue Ying, Yinwei Cao, Pengxiang Xu, Guo Tang, Yufen Zhao
Correction for ‘Metal-free visible-light-induced phosphorylation of unactivated alkyl iodides with white phosphorus as the P-atom source’ by Fushan Chen et al., Green Chem., 2023, 25, 6629–6634, https://doi.org/10.1039/D3GC01579C.
对 Fushan Chen 等人 "以白磷为 P 原子源的无金属可见光诱导的未活化烷基碘化物的磷酸化 "的更正,《绿色化学》,2023 年,25 期,6629-6634,https://doi.org/10.1039/D3GC01579C。
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引用次数: 0
Visible-light-induced hydroxycarboxylation of α-trifluoromethylstyrenes to construct densely functionalized α-CF3 tertiary alcohols 可见光诱导 α-三氟甲基苯乙烯羟基羧化,构建致密官能化 α-CF3 叔醇
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-04 DOI: 10.1039/d4gc01676a
Min-Ming Lu, Ning Deng, Shi-Yu Li, Ren-Jie Tong, Jun Xu, Hua-Jian Xu
A visible-light-induced hydroxycarboxylation of α-trifluoromethylstyrenes is reported herein, which provides a series of α-trifluoromethyl-β-carboxyl tertiary alcohols under mild and environmentally friendly conditions in moderate to good yields. This protocol is enabled by SET between a photocatalyst and sodium formate to obtain CO2˙ without adding an additional HAT reagent. Broad substrate scope, excellent functional group compatibility, gram-scale synthesis and synthetic applications show the significant potential application of this protocol in the synthesis of a variety of compounds with densely functionalized α-CF3 tertiary alcohols.
本文报告了一种可见光诱导的 α-三氟甲基苯乙烯羟基羧化反应,该反应在温和、环保的条件下以中等至良好的产率提供了一系列 α-三氟甲基-β-羧基叔醇。通过光催化剂和甲酸钠之间的 SET,无需添加额外的 HAT 试剂即可获得 CO2˙-。广泛的底物范围、优异的官能团兼容性、克级规模的合成和合成应用表明,该方案在合成各种具有致密官能化 α-CF3 叔醇的化合物方面具有巨大的应用潜力。
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引用次数: 0
C–H fluorination promoted by pyridine N-oxyl radicals 吡啶 N-氧自由基促进的 C-H 氟化作用
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-04 DOI: 10.1039/d4gc02247e
Tianyu Zeng, Chaoqun Huang, Yang Zhang, Yunzi Luo, Dawen Niu
Inspired by C–H hydroxylation by cytochrome P450 enzymes (P450s), we report here a method for preparing organofluorides through a single-electron transfer (SET) process, in which the pyridine N-oxyl radical greatly promotes the C–H fluorination. This reaction can be carried out in pure water at room temperature and accommodates a wide range of substrates, including bioactive molecules, with good yields. Mechanistic investigations indicate that reactions advance through radical intermediates.
受细胞色素 P450 酶(P450)的 C-H 羟基化作用的启发,我们在此报告了一种通过单电子转移(SET)过程制备有机氟化物的方法,其中吡啶 N-氧自由基极大地促进了 C-H 氟化作用。该反应可在室温下的纯水中进行,适用于包括生物活性分子在内的多种底物,而且产率高。机理研究表明,反应是通过自由基中间体进行的。
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引用次数: 0
Low-chromophore lignin isolation from natural biomass with polyol-based deep eutectic solvents 利用多元醇基深共晶溶剂从天然生物质中分离低色团木质素
IF 9.8 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-07-04 DOI: 10.1039/d4gc01824a
Jinyuan Cheng, Xuelian Zhou, Caoxing Huang, Chang Geun Yoo, Xianzhi Meng, Guigan Fang, Arthur J. Ragauskas, Chen Huang
When attempting to obtain light-color lignin from lignocellulosic biomass or industrial lignin, the available options based on chemical or morphological modification suffer from low yield, high cost, and lack of availability at the required scales. In this study, we adopted a polyhydric-alcohol-based deep eutectic solvent (PA-DES) to directly extract light-color lignin from natural biomass, which is even whiter than native cellulolytic enzyme lignin (CEL). The isolated lignin possessed a high recovery yield (97.36%), regular micro-spherical morphology, enriched β-ether linkage of 58/100Ar, low phenolic hydroxyl content of 1.25 mmol g−1, minimal carbonyl content of 0.70 mmol g−1, and less condensed structures, thus yielding a lower content of chromophores. This lignin showed excellent sunscreen effects, which could enhance the SPF of a commercial sunscreen from 15 to 40 with only 5 wt% addition. This study can provide essential guidance for the scale-up production of light-color lignin and obtaining near-complete digestible cellulose for further saccharification.
在尝试从木质纤维素生物质或工业木质素中获取浅色木质素时,现有的基于化学或形态改性的方案都存在产量低、成本高以及缺乏所需规模的可用性等问题。在这项研究中,我们采用基于多羟基乙醇的深共晶溶剂(PA-DES)直接从天然生物质中提取浅色木质素,这种木质素甚至比原生纤维素酶木质素(CEL)更白。分离出的木质素具有较高的回收率(97.36%)、规则的微球状形态、富含 58/100Ar 的 β-醚键、较低的酚羟基含量(1.25 mmol g-1)、极少的羰基含量(0.70 mmol g-1)以及较少的缩合结构,因此产生的发色团含量较低。这种木质素具有出色的防晒效果,只需添加 5 wt%,就能将商用防晒霜的 SPF 值从 15 提高到 40。这项研究为扩大浅色木质素的生产规模和获得近乎完全可消化的纤维素以进一步糖化提供了重要指导。
{"title":"Low-chromophore lignin isolation from natural biomass with polyol-based deep eutectic solvents","authors":"Jinyuan Cheng, Xuelian Zhou, Caoxing Huang, Chang Geun Yoo, Xianzhi Meng, Guigan Fang, Arthur J. Ragauskas, Chen Huang","doi":"10.1039/d4gc01824a","DOIUrl":"https://doi.org/10.1039/d4gc01824a","url":null,"abstract":"When attempting to obtain light-color lignin from lignocellulosic biomass or industrial lignin, the available options based on chemical or morphological modification suffer from low yield, high cost, and lack of availability at the required scales. In this study, we adopted a polyhydric-alcohol-based deep eutectic solvent (PA-DES) to directly extract light-color lignin from natural biomass, which is even whiter than native cellulolytic enzyme lignin (CEL). The isolated lignin possessed a high recovery yield (97.36%), regular micro-spherical morphology, enriched β-ether linkage of 58/100Ar, low phenolic hydroxyl content of 1.25 mmol g<small><sup>−1</sup></small>, minimal carbonyl content of 0.70 mmol g<small><sup>−1</sup></small>, and less condensed structures, thus yielding a lower content of chromophores. This lignin showed excellent sunscreen effects, which could enhance the SPF of a commercial sunscreen from 15 to 40 with only 5 wt% addition. This study can provide essential guidance for the scale-up production of light-color lignin and obtaining near-complete digestible cellulose for further saccharification.","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":null,"pages":null},"PeriodicalIF":9.8,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141547868","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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Green Chemistry
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