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Customized molecular tools to strengthen metabolic engineering of cyanobacteria 加强蓝藻代谢工程的定制分子工具
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.05.002
Stephan Klähn , Franz Opel , Wolfgang R. Hess

Cyanobacteria are promising oxygenic phototrophs for the production of various compounds. For their (photo)biotechnological exploitation, molecular tools are required, such as, for the introduction and expression of heterologous genes, or the modulation of enzyme activities or entire pathways. Concepts and strategies for the development of photosynthetic biomanufacturing technologies based on cyanobacteria have been extensively reviewed, as well as certain specialized aspects of their genetic manipulation. However, options for metabolic engineering of specific cyanobacterial cells are still less developed than those for other bacteria of biotechnological relevance. In addition to the standard genetic toolbox for “classical” metabolic engineering, we emphasize certain aspects, including recently developed vector systems for the extrachromosomal maintenance of genes and approaches based on clustered regularly interspaced short palindromic repeats (CRISPR) interference. We highlight the development of custom molecular tools for specific strains or products, discuss the emerging use of small regulatory proteins that appear promising for advanced metabolic engineering approaches to promote specific product formation, and provide an overview of suitable online resources. Furthermore, we discuss the current trends in this field and indicate their potential, such as using suitable product sensors that enable systematic screening, and optimization approaches.

蓝藻是很有希望生产各种化合物的含氧光养菌。要对其进行(光合)生物技术开发,需要使用分子工具,例如引入和表达异源基因,或调节酶活性或整个途径。以蓝藻为基础开发光合生物制造技术的概念和战略,以及蓝藻遗传操作的某些专门方面,已经得到了广泛的研究。然而,与其他具有生物技术相关性的细菌相比,特定蓝藻细胞的新陈代谢工程方案的开发程度仍然较低。除了用于 "经典 "代谢工程的标准遗传工具箱外,我们还强调了某些方面,包括最近开发的用于染色体外维持基因的载体系统和基于聚类规则间隔短回文重复序列(CRISPR)干扰的方法。我们重点介绍了针对特定菌株或产品的定制分子工具的开发,讨论了新出现的小调控蛋白的使用,这些蛋白似乎有望用于促进特定产品形成的高级代谢工程方法,并概述了合适的在线资源。此外,我们还讨论了这一领域的当前趋势,并指出了其潜力,如使用合适的产品传感器进行系统筛选和优化方法。
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引用次数: 0
Adopting green absorbent for CO2 capture and agricultural utilization: Biogas slurry and biomass ash case 采用绿色吸收剂进行二氧化碳捕获和农业利用:沼气浆和生物质灰案例
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.03.001
Feihong Liang , Shihui Wei , Lu Xue , Shuiping Yan

Previously, the once-through CO2 chemical absorption process by biogas slurry was experimentally verified to offer the unique advantages like low energy consumption, cost-effectiveness, and feasibility of CO2 fixation in plants. However, this technology also faces some challenges and limitations, including a low CO2 absorption rate and performance. To improve the effectiveness and reliability of this innovative carbon capture, utilization, and storage (CCUS) technology, this study proposes a novel method to enhance the CO2 absorption performance without affecting agricultural applications of CO2 by mixing biogas slurry with biomass ash as the green CO2 absorbent. The results indicate that when the solid-liquid mass ratio of biomass ash to biogas slurry is 5:10, the CO2 loading of the biomass ash and biogas slurry mixture (BA-BS) reaches 936.7 ± 59.1 mmol/kg. Furthermore, the pH of the BA-BS remains stable at 6.9, meeting the rhizosphere pH requirements for plant cultivation. The CO2 absorption of the BA-BS liquid phase, referred to as improved biogas slurry (IBS), reaches its maximum at 230.4 ± 3.5 mmol/L, which is 126.8% higher than that of the unimproved biogas slurry. The nitrogen content in the BA-BS solid phase, calling improved biomass ash (IBA), also reaches its maximum at 4.24 ± 0.74 mg/g, thereby expanding the agricultural utilization of biomass ash. The most reasonable and effective way of utilizing CO2-rich mixed biogas slurry and biomass ash involves use IBA as the base fertilizer for tomato cultivation, supplemented later with IBS to promote growth. This optimal application allows for substantial utilization of CO2, introduced into the tomato cultivation environment by IBA and IBS. The carbon fixation of a single tomato has improved by 108.2%. This study thus provides a feasible solution for high-value negative carbonization of biogas slurry and biomass ash.

此前,通过实验验证了沼气浆对二氧化碳的一次性化学吸收过程具有能耗低、成本效益高以及在植物中固定二氧化碳的可行性等独特优势。然而,该技术也面临着一些挑战和限制,包括二氧化碳吸收率低、性能差等。为了提高这种创新型碳捕集、利用和封存(CCUS)技术的有效性和可靠性,本研究提出了一种新方法,通过将沼气浆与生物质灰作为绿色二氧化碳吸收剂混合,在不影响二氧化碳农业应用的前提下提高二氧化碳吸收性能。结果表明,当生物质灰分与沼气浆的固液质量比为 5:10 时,生物质灰分与沼气浆混合物(BA-BS)的二氧化碳负荷达到 936.7 ± 59.1 mmol/kg。此外,BA-BS 的 pH 值稳定在 6.9,符合植物栽培对根瘤菌 pH 值的要求。BA-BS 液相(即改良沼气浆(IBS))的二氧化碳吸收量最大,为 230.4 ± 3.5 mmol/L,比未经改良的沼气浆高出 126.8%。BA-BS 固相中的氮含量也达到最高值,为 4.24 ± 0.74 mg/g,从而扩大了生物质灰的农业利用。利用富含二氧化碳的混合沼气浆和生物质灰渣的最合理、最有效的方法是使用 IBA 作为番茄栽培的基肥,之后再辅以 IBS 以促进生长。这种最佳施肥方式可以大量利用 IBA 和 IBS 引入番茄栽培环境的二氧化碳。单个番茄的碳固定能力提高了 108.2%。因此,这项研究为沼气浆和生物质灰的高价值负碳化提供了一个可行的解决方案。
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引用次数: 0
Size-dependent activity of Fe-N-doped mesoporous carbon nanoparticles towards oxygen reduction reaction 掺杂 Fe-N 的介孔碳纳米颗粒在氧气还原反应中的活性与尺寸有关
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.03.002
Yilun Zhao , Zhengbin Tian , Wenquan Wang , Xiaohui Deng , Jo-Chi Tseng , Guanghui Wang

The rational design of Fe–N–C catalysts that possess easily accessible active sites and favorable mass transfer, which are usually determined by the structure of catalyst supports, is crucial for the oxygen reduction reaction (ORR). In this study, an oleic acid-assisted soft-templating approach is developed to synthesize size-controlled nitrogen-doped carbon nanoparticles (ranging from 130 nm to 60 nm and 35 nm, respectively) that feature spiral mesopores on their surface (SMCs). Next, atomically dispersed Fe–Nx sites are fabricated on the size-tunable SMCs (Fe1/SMC-x, where x represents the SMC size) and the size-dependent activity toward ORR is investigated. It is found that the catalytic performance of Fe1/SMCs is significantly influenced by the size of SMCs, where the Fe1/SMC-60 catalyst shows the highest ORR activity with a half-wave potential of 0.90 V vs. RHE in KOH electrolyte, indicating that the gas-liquid-solid three-phase interface on the Fe1/SMC-60 enhances the accessibility of Fe–Nx sites. In addition, when using Fe1/SMC-60 as the cathode catalyst in aqueous zinc-air batteries (ZABs), it delivers a higher open-circuit voltage (1.514 V), a greater power density (223 mW cm−2), and a larger specific capacity/energy than Pt/C-based counterparts. These results further highlight the potential of Fe1/SMC-60 for practical energy devices associated with ORR and the importance of size-controlled synthesis of SMCs.

Fe-N-C催化剂的合理设计对于氧还原反应(ORR)至关重要,这些催化剂通常由催化剂载体的结构决定,而Fe-N-C催化剂应具有易于获得的活性位点和良好的传质性能。本研究开发了一种油酸辅助软模板方法,用于合成尺寸可控的氮掺杂碳纳米颗粒(分别为 130 纳米至 60 纳米和 35 纳米),其表面具有螺旋介孔(SMC)。接着,在尺寸可调的 SMC(Fe1/SMC-x,其中 x 代表 SMC 尺寸)上制造了原子分散的 Fe-Nx 位点,并研究了其对 ORR 的尺寸依赖性活性。研究发现,Fe1/SMC 的催化性能受到 SMC 大小的显著影响,其中 Fe1/SMC-60 催化剂的 ORR 活性最高,在 KOH 电解液中的半波电位为 0.90 V,相对于 RHE,这表明 Fe1/SMC-60 上的气-液-固三相界面提高了 Fe-Nx 位点的可及性。此外,在水性锌空气电池(ZAB)中使用 Fe1/SMC-60 作为阴极催化剂时,与基于 Pt/C 的催化剂相比,它能提供更高的开路电压(1.514 V)、更大的功率密度(223 mW cm-2)和更大的比容量/能量。这些结果进一步凸显了 Fe1/SMC-60 在与 ORR 相关的实用能源设备方面的潜力,以及尺寸可控的 SMC 合成的重要性。
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引用次数: 0
Advancing AI protein structure prediction and design: From amino acid “bones” to new era of all-atom “flesh” 推进人工智能蛋白质结构预测和设计:从氨基酸 "骨骼 "到全原子 "肉体 "的新时代
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.05.001
Senbiao Fang , Ren Wei , Yinglu Cui , Lin Su
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引用次数: 0
Palladium-catalyzed oxidative double alkoxycarbonylation of ethylene toward succinic acid derivatives 钯催化乙烯氧化双烷氧基羰基化反应生成丁二酸衍生物
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.02.008
Zhi-Peng Bao , Cunyao Li , Li Yan , Yunjie Ding , Xiao-Feng Wu

Employing biodegradable plastics is one of the choices to solve white pollution issues. Polybutylene succinate (PBS), as a biodegradable plastic with good stability and heat resistance, is produced by polymerization of succinic acid and butylene glycol. However, inadequate supply of the direct upstream material succinic acid restricts the development of this industry. In this work, we provide a carbonylative strategy to construct succinic acid derivatives from carbon monoxide (CO), ethylene and alcohols. The reaction catalyzed by palladium catalyst under oxidative conditions.

采用生物降解塑料是解决白色污染问题的选择之一。聚丁二酸丁二醇酯(PBS)是一种生物降解塑料,具有良好的稳定性和耐热性,由丁二酸和丁二醇聚合而成。然而,直接上游材料丁二酸的供应不足限制了这一行业的发展。在这项工作中,我们提供了一种以一氧化碳(CO)、乙烯和醇为原料构建琥珀酸衍生物的羰基化策略。该反应由钯催化剂在氧化条件下催化完成。
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引用次数: 0
Advances in Sn-based oxide catalysts for the electroreduction of CO2 to formate 将二氧化碳电还原为甲酸盐的锡基氧化物催化剂研究进展
Pub Date : 2024-06-01 DOI: 10.1016/j.greenca.2024.03.006
Xiaoyue Tu , Xiangjian Liu , Yu Zhang , Jiawei Zhu , Heqing Jiang

The excessive consumption of fossil fuels increases carbon dioxide (CO2) emissions, and the consequent greenhouse effect resulting from higher levels of this gas in the atmosphere has a significant impact on the environment and climate. This has necessitated the development of environmentally friendly and efficient methods for CO2 conversion. The carbon dioxide electroreduction reaction (CO2RR), which is driven by electricity generated by renewable energy sources (e.g., wind and solar) to convert CO2 into value-added fuels or chemicals, is regarded as a promising prospective path toward carbon cycling. Among the various products, formate, with its relatively simple preparation process, has broad application prospects, and can be used as fuel, hydrogen storage material, and raw material for downstream chemicals. Sn-based oxide electrocatalysts have the advantages of being inexpensive and nontoxic. In addition, these catalysts offer high product selectivity and are regarded as promising catalysts for the electrochemical reduction of CO2 to formate. In this review, we first clarify the reaction mechanisms and factors that influence the reduction of CO2 to formate, and then provide some examples of technologies that could be used to study the evolution of catalysts during the reaction. In particular, we focus on traditional Sn-based oxides (SnO2) and novel Sn-based perovskite oxides that have been developed for use in the field of CO2RR in recent years by considering their synthesis, catalytic performance, optimization strategies, and intrinsic principles. Finally, the current challenges and opportunities for Sn-based oxide electrocatalysts are discussed. The perspectives and latest trends presented in this review are expected to inspire researchers to contribute more efforts toward comprehensively optimizing the performance of the CO2RR to produce formate.

化石燃料的过度消耗增加了二氧化碳(CO2)的排放量,而大气中这种气体含量的升高随之产生的温室效应对环境和气候产生了重大影响。因此,有必要开发环保高效的二氧化碳转化方法。二氧化碳电还原反应(CO2RR)由可再生能源(如风能和太阳能)发电驱动,将二氧化碳转化为高附加值燃料或化学品,被认为是实现碳循环的一条前景广阔的途径。在各种产品中,甲酸酯的制备工艺相对简单,具有广阔的应用前景,可用作燃料、储氢材料和下游化学品的原料。锡基氧化物电催化剂具有价格低廉、无毒等优点。此外,这些催化剂还具有较高的产品选择性,被认为是将 CO2 电化学还原为甲酸盐的理想催化剂。在本综述中,我们首先阐明了二氧化碳还原为甲酸盐的反应机理和影响因素,然后提供了一些可用于研究反应过程中催化剂演变的技术实例。特别是,我们重点介绍了近年来开发用于 CO2RR 领域的传统锡基氧化物(SnO2)和新型锡基过氧化物,考虑了它们的合成、催化性能、优化策略和内在原理。最后,还讨论了当前锡基氧化物电催化剂面临的挑战和机遇。本综述中提出的观点和最新趋势有望激励研究人员为全面优化 CO2RR 生产甲酸盐的性能做出更多努力。
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引用次数: 0
Advances in electrocarboxylation reactions with CO2 二氧化碳电羧化反应的进展
Pub Date : 2024-03-01 DOI: 10.1016/j.greenca.2024.02.001
Junjun Mao , Yubo Wang , Bo Zhang , Yang Lou , Chengsi Pan , Yongfa Zhu , Ying Zhang

Recently, significant research has been conducted on the conversion of carbon dioxide (CO2) into value-added chemicals. With the decreasing cost of clean electricity, electrochemical methods have emerged as potential approaches for converting and fixing CO2. Organic electrochemical synthesis is a promising method for utilizing CO2 because it transforms CO2 into higher-value chemicals. This review introduces the research aspects of CO2 conversion and the mechanisms of CO2 organic electrocarboxylation reactions. Recent progress in electrocarboxylation with CO2 is discussed, considering organic substrates and cathode types under different reaction mechanisms. Finally, the challenges and prospects in this field are highlighted with the aim of further promoting the fundamental understanding of CO2 organic electrocarboxylation.

最近,人们对将二氧化碳(CO2)转化为高附加值化学品进行了大量研究。随着清洁电力成本的降低,电化学方法已成为转化和固定二氧化碳的潜在方法。有机电化学合成是一种很有前景的利用二氧化碳的方法,因为它能将二氧化碳转化为更高价值的化学品。本综述介绍了二氧化碳转化的研究方面以及二氧化碳有机电羧化反应的机理。考虑到不同反应机理下的有机底物和阴极类型,讨论了二氧化碳电羧化的最新进展。最后,强调了该领域的挑战和前景,旨在进一步促进对 CO2 有机电羧化的基本理解。
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引用次数: 0
Monolithic metal-based/porous carbon nanocomposites made from dissolved cellulose for use in electrochemical capacitor 由溶解纤维素制成的单片金属基/多孔碳纳米复合材料用于电化学电容器
Pub Date : 2024-03-01 DOI: 10.1016/j.greenca.2024.01.001
Madhav P. Chavhan , Arjeta Kryeziu , Somenath Ganguly , Julien Parmentier

Porous metal-based carbon nanocomposites, with a monolithic shape, were prepared by a one-pot synthesis from dissolved cellulose and metallic salts using a simple, cheap, and environmentally friendly route. Their potential performances as electrochemical capacitors were tested with three metal precursors (M = Cu, Mn, and Fe) with two loadings and in an asymmetric cell for the Fe-based carbon material. Interestingly, here soluble metal precursors were not deposited on a hard cellulose template but mixed in a precooled concentrated NaOH solution where cellulose was previously dissolved, allowing for a good dispersion of the metallic species. After a freezing step where concomitant cellulose regeneration and pore ice-templating phenomena took place, followed by a carbonization step, the mixture led to a porous carbon monolith embedding well-dispersed metal-based nanoparticles having a diameter below 20 nm and present as metallic, oxide, or carbide phase(s) according to the element M. These materials were characterized by different physicochemical techniques and electrochemical tests. Their performances as supercapacitors are discussed in light of the specific behaviour of the metal-based phase and its influence on the carbon matrix properties such as mesopore formation and carbon graphitization. An asymmetric energy storage cell assembled with a Fe-based carbon electrode against a carbon xerogel electrode derived from a phenolic resin shows specific energy and power of 18.3 Wh kg−1 at 5 mA cm−2 and 1.6 kW kg−1 at 25 mA cm−2, respectively.

采用简单、廉价和环保的方法,以溶解的纤维素和金属盐为原料,通过一锅合成法制备了具有整体形状的多孔金属基碳纳米复合材料。在三种金属前体(M = 铜、锰和铁)的两种负载下,以及在铁基碳材料的非对称电池中,测试了它们作为电化学电容器的潜在性能。有趣的是,这里的可溶性金属前驱体不是沉积在坚硬的纤维素模板上,而是混合在预先溶解了纤维素的预冷浓 NaOH 溶液中,从而使金属物种得到良好的分散。经过冷冻步骤(同时发生纤维素再生和孔隙结冰现象)和碳化步骤后,混合物形成了多孔碳单体,其中嵌入了分散良好的金属基纳米颗粒,其直径小于 20 纳米,根据元素 M 的不同呈现为金属相、氧化物相或碳化物相。根据金属基相的特殊行为及其对碳基质特性(如介孔形成和碳石墨化)的影响,讨论了它们作为超级电容器的性能。用铁基碳电极与酚醛树脂制成的碳 xerogel 电极组装的不对称储能电池在 5 mA cm-2 和 25 mA cm-2 时的比能量和比功率分别为 18.3 Wh kg-1 和 1.6 kW kg-1。
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引用次数: 0
Carbon nanotube-based photothermal membrane for efficient cold air heating and removal of particulate matter and airborne bacteria 基于碳纳米管的光热膜,用于高效冷空气加热和去除颗粒物及空气中的细菌
Pub Date : 2024-03-01 DOI: 10.1016/j.greenca.2023.12.002
Weichao Dong , Lina Huang , Xiangju Song , Yan Zhang , Mengke Liu , Zhenzhen Ren , Long Pang , Hui Peng , Heqing Jiang

Indoor heating results in high energy consumption and severe atmospheric pollution. Although the development of solar air heaters provides a sustainable route for indoor thermal comfort, such heaters still face challenges in terms of adequate heat exchange and filtering of atmospheric pollutants. Inspired by solar-driven interfacial evaporation, we propose a multifunctional carbon nanotube-based photothermal membrane for efficient cold air heating and purification via ventilation. Carbon nanotubes endow the membrane with high light absorption and thermal conversion capabilities, thereby sufficiently heating the approaching cold air. With the hierarchical structure formed by phase inversion, the thin upper skin of the composite membrane intercepts micropollutants via the size-sieving effect, whereas the finger-like pores and interpenetrating macrovoids inside the membrane ensure that the heated clear air passes through quickly. A proof-of-principle experiment indicated a cold airflow of 1 L/min across the membrane, yielding a temperature increase of ca. 37 °C as well as a PM 2.5 rejection always higher than 93%. Further antibacterial experiments demonstrated that the membrane effectively removed airborne bacteria. This multifunctional carbon nanotube-based photothermal membrane with specific microstructures not only improves the indoor living quality but also provides a sustainable development scheme to coordinate the relationship among energy utilization, building heating, and air purification.

室内供暖导致高能耗和严重的大气污染。尽管太阳能空气加热器的开发为室内热舒适提供了一条可持续发展的途径,但此类加热器在充分热交换和过滤大气污染物方面仍面临挑战。受太阳能驱动的界面蒸发的启发,我们提出了一种基于碳纳米管的多功能光热膜,用于高效冷空气加热和通风净化。碳纳米管赋予了该膜很高的光吸收和热转换能力,从而可以充分加热临近的冷空气。通过相位反转形成的分层结构,复合膜上层的薄表皮可通过尺寸筛分效应拦截微污染物,而膜内的指状孔隙和相互渗透的大空腔则可确保加热后的清澈空气快速通过。原理验证实验表明,1 升/分钟的冷气流通过薄膜时,温度上升约 37 °C,PM2.5 阻隔率始终高于 93%。进一步的抗菌实验表明,该膜能有效去除空气中的细菌。这种具有特殊微结构的多功能碳纳米管光热膜不仅能改善室内生活质量,还为协调能源利用、建筑供暖和空气净化之间的关系提供了一种可持续发展方案。
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引用次数: 0
Recycled polymer: Green roads for polyester plastics 再生聚合物:聚酯塑料的绿色之路
Pub Date : 2024-03-01 DOI: 10.1016/j.greenca.2024.01.004
Rulin Yang , Guangqiang Xu , Wenjie Tao , Qinggang Wang , Yong Tang

Plastics are integral to numerous significant social advancements. Nonetheless, their contribution to environmental pollution and climate crises cannot be disregarded, as their negative impact on the environment increases with incremental production capacity and demand. Concerted global action is urgently required to promote the green recycle of plastics to prevent their accumulation in the environment and mitigate carbon emissions. This review aims to reveal the paths of green development for polyester plastics, incorporating the trends of the green revolution in mature commercial polyester plastics, newly emerging biodegradable polyester plastics, and future polyester plastics. A critical discussion was conducted on the current and potential future research areas from multiple perspectives, including raw materials, processes, and recycling, to propel us into a future marked by sustainability.

塑料是众多重大社会进步的组成部分。然而,塑料对环境污染和气候危机的影响不容忽视,因为随着生产能力和需求的增加,塑料对环境的负面影响也在增加。全球迫切需要采取一致行动,促进塑料的绿色循环利用,以防止其在环境中积累并减少碳排放。本综述旨在揭示聚酯塑料的绿色发展之路,包括成熟商业聚酯塑料、新兴生物降解聚酯塑料和未来聚酯塑料的绿色革命趋势。从原材料、工艺和回收利用等多个角度对当前和未来潜在的研究领域进行了深入探讨,以推动我们迈向可持续发展的未来。
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引用次数: 0
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