Current Opinion in Green and Sustainable Chemistry最新文献

英文中文

Tandem plasma electrocatalysis: An emerging pathway for sustainable ammonia production 串联等离子体电催化：可持续氨生产的新兴途径

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100986

Weitao Wang , Yaolin Wang , Xin Tu

The Haber-Bosch process, the dominant process for industrial ammonia production, is highly energy-intensive and a major source of carbon emissions. Plasma and electrocatalysis offer viable and promising alternatives for nitrogen reduction reactions, especially when integrated with intermittent renewable electricity. However, relying solely on plasma or electrocatalysis for direct N₂ reduction presents significant challenges. Plasma technology suffers from low conversion efficiency and high energy consumption. Similarly, electrocatalysis encounters challenges with low yield and Faradaic efficiency, primarily due to the low solubility of nitrogen gas and interference of the competing hydrogen evolution reaction. A tandem process combining plasma synthesis of NO_x (a mixture of NO and NO₂) with the electrochemical NO_x reduction reaction (eNO_x⁻RR) can effectively use NO_x as an intermediate, thereby significantly reducing the difficulty of N₂ activation in plasma and enhancing the Faradaic efficiency of the subsequent electrocatalytic process. This promising solution has great potential to dramatically enhance the ammonia synthesis rate, making the tandem process a compelling technology for sustainable and decentralized ammonia synthesis under mild conditions. This review provides an insightful overview of the tandem plasma-electrocatalytic process, illustrating the reported methods for plasma-driven nitrogen activation to nitrogen oxides and discussing the recent advances and challenges in eNO_x⁻RR, with a particularly focus on developing efficient electrocatalysts. Additionally, we discuss the systemic challenges of integrating these two processes, highlighting the importance of process optimization and the potential for ammonia production. The techno-economic and environmental impacts of the tandem process are also evaluated and compared to the Haber-Bosch process, providing insights into future development pathways for this innovative approach.

哈伯-博世工艺是工业氨生产的主要工艺，它是高度能源密集型的，也是碳排放的主要来源。等离子体和电催化为氮还原反应提供了可行且有前途的替代方案，特别是当与间歇性可再生电力相结合时。然而，仅仅依靠等离子体或电催化来直接减少N₂存在很大的挑战。等离子体技术存在转换效率低、能耗高的问题。同样，电催化也面临产率低和法拉第效率低的挑战，这主要是由于氮气的溶解度低和竞争性析氢反应的干扰。将等离子体合成NOx （NO和NO2的混合物）与电化学NOx还原反应（eNOx−RR）串联起来，可以有效地利用NOx作为中间体，从而显著降低了等离子体中N2的活化难度，提高了后续电催化过程的法拉第效率。这种有希望的解决方案具有极大的潜力，可以显着提高氨合成速率，使串联工艺成为一种在温和条件下可持续和分散的氨合成技术。这篇综述对串联等离子体电催化过程进行了深刻的概述，说明了等离子体驱动氮活化成氮氧化物的方法，并讨论了eNOx - RR的最新进展和挑战，特别侧重于开发高效的电催化剂。此外，我们讨论了整合这两个过程的系统性挑战，强调了过程优化的重要性和氨生产的潜力。对串联工艺的技术经济和环境影响进行了评估，并与Haber-Bosch工艺进行了比较，为这种创新方法的未来发展路径提供了见解。

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引用次数: 0

Plasma fluidized beds and their scalability 等离子流化床及其可扩展性

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100984

Tomohiro Nozaki , Xiaozhong Chen , Dae-Yeong Kim , Hyun-Ha Kim

Over the last decade, plasma catalysis has attracted considerable research attention as an emerging low-carbon technology. In plasma catalysis, stable molecules such as CO₂, CH₄, and N₂ are activated by electron impact or electrical energy, thereby ushering in a low-temperature chemistry domain that departs from energy-intensive, heat-dependent systems. Moreover, renewable-energy-driven plasma technologies are expected to help realize power-to-X schemes. In this short review, fluidized bed (FB) reactors incorporated with dielectric barrier discharge (DBD) are explored as potential candidates for upscaling plasma catalysis systems without employing a numbering-up approach. To that end, a scaled-up FB-DBD reactor is conceptualized using CO₂ methanation as a model reaction, followed by the validation of laboratory-scale FB-DBD reactors, which exhibit remarkably high feed gas conversion rates at temperatures lower than those of thermal catalysis units. Finally, certain salient conclusions and perspectives are presented.

在过去的十年中，等离子体催化作为一种新兴的低碳技术引起了广泛的研究关注。在等离子体催化中，稳定的分子如CO2、CH4和N2被电子冲击或电能激活，从而进入一个低温化学领域，与能量密集、热依赖的系统不同。此外，可再生能源驱动的等离子体技术有望帮助实现power-to-X计划。在这篇简短的综述中，结合介质阻挡放电（DBD）的流化床（FB）反应器作为升级等离子体催化系统的潜在候选者进行了探讨，而不采用编号方法。为此，以CO2甲烷化为模型反应，对放大的FB-DBD反应器进行了概念化，随后对实验室规模的FB-DBD反应器进行了验证，该反应器在低于热催化装置的温度下表现出显着的高原料气转化率。最后，提出了一些重要的结论和观点。

引用次数: 0

Ancestral cuisine as regenerative social technologies in Amazon: Eco-humanist perspectives towards a critical sustainable chemistry 祖传美食在亚马逊作为再生社会技术：生态人文主义的观点对一个关键的可持续化学

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2025.101006

Aymara Llanque Zonta , Vânia G. Zuin Zeidler

“Ancestral cuisine” is a reflection from the regenerative agriculture to the culinary, to exemplify the integral relationships between nature and culture, based on the food preparation and consumption practices of indigenous and peasant populations. Socio-scientific studies were taken as a reference, and other secondary sources around the Amazon, especially in northern Peru, Colombia, and Brazil, where conventional monoculture food systems coexist with more traditional forms of food production and consumption. Based mainly on the experiences of women cooks, their culinary and the knowledge transmission, we review and discuss the social technologies and the chemical processes involved, as a starting point of food sustainability criteria to contribute to the ontological shift in the human-nature relationship.

“祖传美食”是一种从再生农业到烹饪的反映，以土著和农民人口的食物制备和消费实践为基础，体现了自然与文化之间的整体关系。社会科学研究作为参考，并参考了亚马逊周围的其他二手资料，特别是在秘鲁北部、哥伦比亚和巴西，传统的单一种植粮食系统与更传统的粮食生产和消费形式共存。主要基于女性厨师的经验，她们的烹饪和知识传播，我们回顾和讨论了社会技术和化学过程所涉及的，作为食物可持续性标准的起点，有助于人与自然关系的本体论转变。

引用次数: 0

Eugenol's journey to high-performance and fire-retardant bio-based thermosets 丁香酚的高性能和阻燃生物基热固性材料之旅

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100988

Pierre Delliere, Camille Bakkali-Hassani, Sylvain Caillol

引用次数: 0

Primary and secondary waste in (bio)catalysis: What matters is not what is produced but what permanently remains! （生物）催化中的初级和次级废物：重要的不是产生什么，而是永久留下什么！

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2025.101003

Pablo Domínguez de María

(Bio)catalysis creates waste, composed of wastewater and an organic fraction. Different metrics are used for the environmental impact of processes, being E-Factor and process mass intensity (PMI) the prominent ones. These metrics are typically applied to wastewater and spent organic fraction, which is the process “Primary Waste.” However, “Primary Waste” is industrially treated before it is released to the environment. When treating “Primary Waste,” CO₂ is generated, from the wastewater treatment plant and from the organic fraction incineration. That CO₂, coined as “Secondary Waste,” remains in the planet and thus should be the target for environmental assessments. When E-Factor and PMI calculated from “Primary Waste” are compared to the values of produced CO₂, results mismatch because the CO₂ depends on the proportion wastewater/organic fraction since incineration leads to higher CO₂ production than wastewater treatment. Sustainable options for (bio)catalysis would be process intensification, incorporating renewable energy and biogenic solvents (neutral carbon), and developing (new) wastewater treatment strategies to deliver pure(r) water effluents to the environment.

（生物）催化产生由废水和有机组分组成的废物。不同的指标用于过程的环境影响，其中e因子和过程质量强度（PMI）是突出的两个。这些指标通常应用于废水和废有机部分，这是“初级废物”的过程。然而，“初级废物”在排放到环境之前是经过工业处理的。当处理“初级废物”时，从废水处理厂和有机部分焚烧产生二氧化碳。被称为“二次废物”的二氧化碳仍然留在地球上，因此应该成为环境评估的目标。当从“初级废物”中计算出的E-Factor和PMI与产生的CO2值进行比较时，结果不匹配，因为CO2取决于废水/有机组分的比例，因为焚烧导致的CO2产生量高于废水处理。（生物）催化的可持续选择将是过程强化，纳入可再生能源和生物溶剂（中性碳），并制定（新的）废水处理战略，向环境排放纯（或）废水。

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引用次数: 0

Applying the principles of green chemistry to achieve a more sustainable polymer life cycle 应用绿色化学原理实现更可持续的聚合物生命周期

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100996

Francesca M. Kerton

This mini-review highlights how many of the principles of green chemistry can be used to make polymers more sustainable. The use of renewable feedstocks has grown enormously in the recent years including the use of bio-derived monomers and modifications of natural polymers such as carbohydrates. Polymers are also being designed to allow entry into the circular economy especially where triggered depolymerization (e.g. catalytic recycling to monomer) can occur, which can allow easy separation from other plastics in a mixed waste stream. Computational studies and reaction monitoring are useful in identifying and understanding reactivity trends for polymer synthesis and degradation. Solvent-free reactions, including mechanochemistry, can be employed to reduce process mass intensity and environmental impacts. Use of standard polymer degradation conditions (e.g. ISO standards) and life-cycle assessments, in particular hot spot analyses, should be encouraged in order to accelerate progress in this important field.

这篇小型综述强调了绿色化学的许多原理可以用来使聚合物更具可持续性。近年来，可再生原料的使用急剧增长，包括使用生物衍生单体和天然聚合物（如碳水化合物）的改性。聚合物也被设计为允许进入循环经济，特别是在可以发生触发解聚（例如催化回收到单体）的地方，这可以使混合废物流中的其他塑料容易分离。计算研究和反应监测对于识别和理解聚合物合成和降解的反应性趋势是有用的。无溶剂反应，包括机械化学，可以用来减少过程质量强度和环境影响。应鼓励使用标准聚合物降解条件（例如ISO标准）和生命周期评估，特别是热点分析，以便加速这一重要领域的进展。

引用次数: 0

Process-chemistry intensification using non-thermal plasmas: Toward one-step chemical production 使用非热等离子体的过程化学强化：迈向一步化学生产

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2025.100997

Nefeli S. Kamarinopoulou , Darien K. Nguyen , Dionisios G. Vlachos

Decarbonizing the chemical industry requires process electrification. Non-thermal plasmas present an electrification alternative to fossil fuel-based thermal chemistry due to their modularity, fast dynamics, and compatibility with renewable energy sources. Their most remarkable quality is the non-equilibrium state between molecules and high-energy electrons, enabling molecular activation at mild conditions. Unlike chemical manufacturing constrained by thermal activation, limiting feedstock options and necessitating multistep processes, plasma electron impact excitation can open direct (one step) chemical synthesis. We highlight the potential of plasmas from the perspective of process-chemistry intensification.

化学工业脱碳需要过程电气化。非热等离子体由于其模块化、快速动力学和与可再生能源的兼容性，为化石燃料的热化学提供了一种电气化替代方案。它们最显著的特点是分子和高能电子之间的非平衡状态，使分子在温和的条件下激活。不像化学制造受到热活化的限制，限制原料选择和需要多步骤的过程，等离子体电子冲击激发可以打开直接（一步）化学合成。我们从过程化学强化的角度强调了等离子体的潜力。

引用次数: 0

The active facet of copper and its alloy for selective and efficient electrochemical reduction of nitrate to ammonia 铜及其合金选择性高效电化学还原硝态氮的活性面

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100995

Kartick Chandra Majhi , Zehui Zhang , Feng Chunhua , Yang Lei , Jason Chun-Ho Lam

Electrochemical reduction of nitrate (NO₃⁻) to ammonia (NH₃) (the e-NO₃RR) is one of the most widely discussed methods to remediate the NO₃⁻ concentrations found in industrial and agricultural wastewater. The growing importance of NH₃ stems from its central role in fertilizer and advanced chemical production and as an emerging renewable hydrogen carrier due to its excellent hydrogen ratio and liquefiability.

This review highlights how the active facets of copper (Cu), the most widely documented electrocatalyst for e-NO₃RR, and its alloys transform NO₃⁻ to NH₃. The literature findings on Faradaic efficiency and the NH₃ formation rate in connection with the Cu facet, Cu oxide, and Cu alloys are discussed, followed by a discussion of the potential opportunities of the e-NO₃RR. We hope this review will provide helpful information to facilitate the design of the next generation of electrocatalysts.

电化学还原硝态氮（NO3−）为氨（NH3）（e-NO3RR）是修复工农业废水中NO3−浓度的最广泛讨论的方法之一。NH3在化肥和先进化工生产中的核心作用，以及由于其优异的氢比和可液化性而成为新兴的可再生氢载体，因此其重要性日益增加。这篇综述强调了铜（Cu）的活性方面，最广泛记录的e-NO3RR电催化剂，及其合金将NO3−转化为NH3。讨论了与Cu面、Cu氧化物和Cu合金有关的Faradaic效率和NH3生成速率的文献发现，然后讨论了e-NO3RR的潜在机会。希望本文的综述能为下一代电催化剂的设计提供有益的信息。

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引用次数: 0

Fundamental insights and emerging opportunities in plasma catalysis for light alkane conversion 等离子体催化轻烷烃转化的基本见解和新机会

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100987

Denver J. Haycock , Russell J. Clarke , David B. Go , William F. Schneider , Jason C. Hicks

With increasingly available renewable sources of electricity, plasma catalysis could be a key component in the decarbonization of natural gas and greenhouse gas valorization. Fundamental insight is needed in both the coupling of plasma and catalytic chemistries, and in chemical limitations and opportunities of such coupled systems to enable larger scale engineering and optimization. This perspective describes some of the pressing needs and high-impact opportunities present in the current research landscape of plasma catalysis for light hydrocarbons.

随着越来越多的可再生电力，等离子体催化可能是天然气脱碳和温室气体增值的关键组成部分。等离子体和催化化学的耦合，以及这种耦合系统的化学限制和机会，都需要基本的洞察力，以实现更大规模的工程和优化。这一观点描述了目前轻烃等离子体催化研究领域的一些迫切需求和高影响力的机会。

引用次数: 0

Recent progresses of plasma-catalytic CH4/CO2 conversion to oxygenates: A short review 等离子体催化CH4/CO2转化为氧合物的研究进展

IF 9.3 2区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Current Opinion in Green and Sustainable Chemistry

Pub Date : 2025-02-01 DOI: 10.1016/j.cogsc.2024.100989

Li Wang , Qingxi Yin , Xiaohan Zhai , Yanhui Yi

Plasma catalysis is a promising alternative for the direct conversion of CO₂ and CH₄ to high-value oxygenates at mild conditions. However, this direct process suffers from low selectivity and high diversity of the liquid oxygenates, generally consisting of C_1-4 alcohols, C_1-2 acids, C_1-2 aldehydes and acetone, and little is known yet about how to selectively produce one target oxygenate. The trial-and-error approach still dominates the current researches, especially in screening effective catalysts. This short review highlights researches in the last two years, revealing the crucial factors that affect oxygenates formation, and then proposing some feasible strategies to improve oxygenates formation in plasma-catalytic CO₂/CH₄ conversion.

等离子体催化是在温和条件下将CO2和CH4直接转化为高值氧化物的一种有前途的替代方法。然而，这种直接制程存在液态氧合物选择性低、多样性高的问题，通常由C1-4醇类、C1-2酸类、C1-2醛类和丙酮类组成，如何选择性地生成一种目标氧合物尚不清楚。试错法在目前的研究中仍然占主导地位，特别是在筛选有效催化剂方面。本文简要回顾了近两年的研究成果，揭示了影响氧合物形成的关键因素，并提出了改善等离子体催化CO2/CH4转化过程中氧合物形成的可行策略。

引用次数: 0

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全部 ACS Publications Elsevier ieeexplore Springer The Royal Society of Chemistry Wiley

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Current Opinion in Green and Sustainable Chemistry

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