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Recent advances in catalytic hydroprocessing of lignin and plastics for aromatic compound production 木质素和塑料催化加氢生产芳香族化合物的研究进展

Green Carbon

Pub Date : 2025-12-01 DOI: 10.1016/j.greenca.2025.05.003

Haoquan Guo , Xinyi Zhang , Yuguo Dong , Jiaxin Liu , Xiaoli Gu , Yihu Dai , Yu Tang

Lignin and plastics are two of the most extensively used polymeric materials in contemporary industrial systems. As a biomass-derived polymer containing abundant aromatic units, lignin has emerged as a prime candidate for replacing fossil fuels owing to its renewable nature. Paradoxically, as synthetic polymer materials with aromatic structures similar to those of lignin, plastics have become a critical environmental challenge owing to their accumulation over recent decades. The inherent stabilities of lignin and plastics pose significant challenges for their efficient utilization and recycling, making catalytic depolymerization a focal research point in recent years. Innovative catalytic strategies that enable the high-yield production of aromatic compounds through the catalytic hydroprocessing of lignin and plastic waste have recently emerged. These methods offer opportunities for the conversion of recalcitrant polymers into valuable chemicals and sustainable fuels. This paper comprehensively reviews these advancements and emphasizes their potential applications in catalytic hydroprocessing for biofuel production. Additionally, it highlights the latest developments in the high-value upgrading of lignin derivatives and underscores their significance in building a sustainable chemical industry. The review examines the entire value chain from lignin and plastic depolymerization to the production of high-value chemicals to outline the potential for enhancing the efficiency of sustainable processes. This emphasizes the critical role of developing novel cost-effective methodologies for the catalytic depolymerization of lignin and plastic waste. These advancements are expected to play a pivotal role in fostering a sustainable economy and addressing pressing environmental challenges.

木质素和塑料是当代工业系统中使用最广泛的两种高分子材料。木质素作为一种含有丰富芳香族单元的生物质衍生聚合物，由于其可再生特性，已成为替代化石燃料的主要候选材料。矛盾的是，作为与木质素类似的芳香族结构的合成聚合物材料，塑料在近几十年来的积累已经成为一个关键的环境挑战。木质素和塑料的固有稳定性对其有效利用和回收提出了重大挑战，催化解聚成为近年来的研究热点。最近出现了创新的催化策略，使木质素和塑料废物的催化加氢处理能够高产出芳香族化合物。这些方法为将顽固性聚合物转化为有价值的化学品和可持续燃料提供了机会。本文对这些进展进行了综述，并强调了它们在生物燃料催化加氢加工中的潜在应用。此外，它还重点介绍了木质素衍生物的高价值升级的最新进展，并强调了它们在建设可持续化学工业中的重要性。该审查审查了从木质素和塑料解聚到高价值化学品生产的整个价值链，以概述提高可持续过程效率的潜力。这强调了开发新的具有成本效益的木质素和塑料废物催化解聚方法的关键作用。预计这些进步将在促进可持续经济和应对紧迫的环境挑战方面发挥关键作用。

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引用次数: 0

Landscape profiling method for mining novel PET hydrolases: Advances and industrial implications 利用景观剖面法开采新型PET水解酶：进展及其工业意义

Green Carbon

Pub Date : 2025-12-01 DOI: 10.1016/j.greenca.2025.05.001

Yi Zheng, Tianyuan Su, Qingsheng Qi

引用次数: 0

Machine learning models for rapid prediction of chemicals’ life-cycle environmental impacts: Current status, challenges, and future directions 用于快速预测化学品生命周期环境影响的机器学习模型：现状、挑战和未来方向

Green Carbon

Pub Date : 2025-12-01 DOI: 10.1016/j.greenca.2025.05.004

Kai Zhao , Xiting Peng , Shanying Hu , Xiaonan Wang

Understanding and reducing the life-cycle environmental impacts of chemicals can benefit a wide range of industries. However, current life cycle assessments (LCA) of chemicals are limited by slow speed and high cost. Molecular-structure-based machine learning (ML) is the most promising technology for the rapid prediction of life-cycle environmental impacts of chemicals. Advances in training datasets, feature engineering, and model architectures for ML models in this area are systematically discussed in this review. We call for the establishment of a large, open, and transparent LCA database for chemicals that includes a wider range of chemical types to address the challenge of data shortages. Greater emphasis on external regulation of data is also needed to produce high-quality LCA data. The construction of more efficient chemical-related descriptors and the identification of features most pertinent to LCA results represent pivotal steps in the advancement of next-generation modeling. The integration of large language models (LLMs) is expected to provide new impetus for database building and feature engineering. Finally, expanding the dimensions of predictable chemical life cycles can further extend the applicability of relevant research. This review aims to outline key strategies to advance this emerging field.

了解和减少化学品的生命周期对环境的影响可以使许多行业受益。然而，目前的化学品生命周期评估存在着速度慢、成本高的问题。基于分子结构的机器学习（ML）是快速预测化学物质生命周期环境影响的最有前途的技术。本文系统地讨论了在该领域中机器学习模型的训练数据集、特征工程和模型架构方面的进展。我们呼吁建立一个大型、开放和透明的化学品LCA数据库，包括更广泛的化学品类型，以应对数据短缺的挑战。为了产生高质量的LCA数据，还需要更加强调数据的外部监管。构建更有效的化学相关描述符和识别与LCA结果最相关的特征是下一代建模进步的关键步骤。大型语言模型（llm）的集成有望为数据库构建和特征工程提供新的动力。最后，扩大可预测化学生命周期的维度，可以进一步扩展相关研究的适用性。本综述旨在概述推进这一新兴领域的关键战略。

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引用次数: 0

Rational design of d-hydantoinase from Pseudomonas aeruginosa for desymmetric synthesis of chiral intermediate for (S)-pregabalin 铜绿假单胞菌d-羟酶的合理设计，用于不对称合成(S)-普瑞巴林的手性中间体

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2025.02.002

Feixia Liu , Huili Zhao , Zhongdong Shang , Fa Zhang , Tristan de Rond , Bo Yu

(S)-Pregabalin (S-PGB) is extensively employed in analgesic therapy. One of the current chemical processes used to produce S-PGB involves the Hofmann rearrangement of (R)-3-isobutyl glutaric acid monoamide (R-IBM). However, the chemical resolution of R-IBM is inefficient and environmentally unsustainable. In this study, we established an enzyme-catalyzed route to R-IBM that proceeds with exceptional optical purity and yield. We successfully resculpted the substrate-binding pocket of d-hydantoinase by attenuating the steric hindrance and enhancing hydrophilicity, resulting in accelerated substrate transport and restricted side-chain rotation during the asymmetric hydrolysis process. Notably, both optical purity and yield for the generation of R-IBM from the prochiral substrate 3-isobutyl glutarimide (IBI) were enhanced for the M3 (L64A/F66H/C318T) mutant; the enantiomeric excess increased from 65.51 % ± 5.85 % to 98.62 %± 0.28 % (ee_p) and k_cat/K_m increased from 14.92 to 207.06 s⁻¹∙M⁻¹. The ancestral sequence reconstruction (ASR) and consensus analyses guided further engineering of the flexible C-terminal region of d-hydantoinase to enhance the thermostability of the enzyme. The final mutant, M6 (L64A/F66H/C318T/R99G/A265P/G466N/E470A), demonstrated a remarkable improvement in R-IBM production efficiency; thus, 500 mM IBI was completely transformed into R-IBM in 24 h. This study therefore showcases a new enzyme that offers a green, enzymatic route for R-IBM production.

(S)-普瑞巴林（S- pgb）广泛应用于镇痛治疗。目前用于生产S-PGB的化学工艺之一涉及(R)-3-异丁基戊二酸单酰胺（R- ibm）的霍夫曼重排。然而，R-IBM的化学解析度效率低下，而且在环境上不可持续。在这项研究中，我们建立了一种酶催化的R-IBM途径，该途径具有优异的光学纯度和收率。通过减小位阻和增强亲水性，我们成功地重塑了d-羟酶的底物结合袋，从而在不对称水解过程中加速了底物运输和限制了侧链旋转。值得注意的是，M3 （L64A/F66H/C318T）突变体从前手性底物3-异丁基戊二酰亚胺（IBI）生成R-IBM的光学纯度和产量都得到了提高；对映体过量从65.51 % ± 5.85 %增加到98.62 %± 0.28 % (eep)， kcat/Km从14.92增加到207.06 s−1∙M−1。祖先序列重建（ASR）和共识分析指导了d-羟化酶柔性c端区域的进一步工程设计，以提高酶的热稳定性。最终突变体M6 （L64A/F66H/C318T/R99G/A265P/G466N/E470A）的R-IBM生产效率显著提高；因此，500 mM IBI在24 h内完全转化为R-IBM。因此，这项研究展示了一种新的酶，为R-IBM生产提供了绿色的酶途径。

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引用次数: 0

Revolutionizing unsymmetrical urea synthesis: A bimetallic catalytic approach with synchronous recognition mechanism 革新不对称尿素合成：具有同步识别机制的双金属催化方法

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2024.12.002

Zechao Wang

引用次数: 0

Dual piezoelectric catalytic system for efficient CO2 reduction 双压电催化系统，高效二氧化碳还原

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2025.01.005

Yu Luo , Jie Wang , Hui Li , Ying Sun , Qin Zhao , Tianyi Ma

In the pursuit of sustainable carbon dioxide (CO₂) reduction strategies, this study explores the potential of a novel dual piezoelectric system comprising K_0.5Na_0.5NbO₃ (KNN) and polyvinylidene fluoride-hexafluoropropylene (PVDF-HFP) for enhanced CO₂ catalytic reduction. The dual piezoelectric coating fabricated using a simple and adjustable method demonstrated remarkable versatility in applications to diverse surfaces and shapes. This system not only amplifies piezoelectric carrier generation but also enhances carrier separation and transfer through the synergistic effect of the dual piezoelectric materials. The integration of acetylene black further improves the conductivity and optimizes the piezoelectric catalytic performance. Under optimal conditions, the composite film achieves a significant carbon monoxide (CO) yield of 191.6 μmol g⁻¹ h⁻¹, representing a 13-fold enhancement over pure KNN. In addition, we investigated the underlying piezoelectric catalytic mechanism, revealing the critical role of the band structure and polarization fields in facilitating CO₂ reduction. This work not only underscores the effectiveness of the dual piezoelectric system but also paves the way for the development of high-performance piezoelectric catalysts with broad industrial applications, advancing the field of piezoelectric catalysis for more sustainable CO₂ reduction technologies.

为了追求可持续的二氧化碳（CO2）减排策略，本研究探索了一种新型双压电系统的潜力，该系统由K0.5Na0.5NbO3 （KNN）和聚偏氟乙烯-六氟丙烯（PVDF-HFP）组成，用于增强二氧化碳催化还原。采用简单可调的方法制备的双压电涂层在不同表面和形状的应用中表现出显著的多功能性。该系统不仅放大了压电载流子的产生，而且通过双压电材料的协同作用增强了载流子的分离和转移。乙炔黑的集成进一步提高了电导率，优化了压电催化性能。在最佳条件下，复合膜的一氧化碳（CO）产率达到了191.6 μmol g−1 h−1，比纯KNN提高了13倍。此外，我们还研究了潜在的压电催化机制，揭示了能带结构和极化场在促进CO2还原中的关键作用。这项工作不仅强调了双压电系统的有效性，而且为开发具有广泛工业应用的高性能压电催化剂铺平了道路，推动了压电催化领域更可持续的二氧化碳减排技术。

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引用次数: 0

Porous materials with terminal zinc hydride sites to capture high-temperature carbon dioxide 具有末端氢化锌位点的多孔材料，用于捕获高温二氧化碳

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2025.03.001

Zhuoshen Huang , Wei Xia , Xiubing Huang

引用次数: 0

Adipic acid synthesis from bio-derived 2-furoic acid by reduction-carbonylation 生物源2-呋喃酸羰基化还原合成己二酸

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2025.02.008

Changpo Ma , Tiange Zhao , Xiaoxuan Zhang , Shiyu Shen , Yunpu Wang , Lingzhao Kong , Weiran Yang

Adipic acid (ADA) serves as a crucial monomer for the manufacturing of nylon and polyurethanes. However, current production methods are based on petrochemical feedstocks and pose significant environmental concerns. Consequently, the development of an innovative catalytic system for producing ADA from renewable biomass-derived feedstocks is of significant importance. Herein, we report a novel one-pot, two-step process for the highly efficient synthesis of ADA from the biomass derivative 2-furoic acid via hydrogenative carbonylation. In the first step, 2-furoic acid is selectively reduced to 2-tetrahydrofuroic acid using a Rh catalyst with acetic acid (AcOH) and water (H₂O) as solvents. Subsequently, within the same catalytic system, the addition of I₂ as a promoter enables the further conversion of 2-tetrahydrofuroic acid to ADA through a highly selective carbonylation reaction under CO and H₂ atmospheres. This one-pot, two-step process achieved an ADA yield of 91.4 % from 2-furoic acid. Mechanistic studies revealed that 5-iodopentanoic acid is the key intermediate in the carbonylation process. In summary, this research introduces an innovative and environmentally friendly approach for synthesizing ADA from biomass-derived 2-furoic acid, offering great potential for industrial application.

己二酸（ADA）是制造尼龙和聚氨酯的关键单体。然而，目前的生产方法是基于石化原料，造成严重的环境问题。因此，开发一种创新的催化系统，从可再生生物质来源的原料中生产ADA是非常重要的。在此，我们报告了一种新的一锅，两步的方法，以生物质衍生物2-呋喃酸为原料，通过氢化羰基化高效合成ADA。第一步，以乙酸（AcOH）和水（H2O）为溶剂，采用Rh催化剂选择性地将2-呋喃二酸还原为2-四氢呋喃二酸。随后，在相同的催化体系中，加入I2作为促进剂，使2-四氢呋喃酸在CO和H2气氛下通过高选择性羰基化反应进一步转化为ADA。这一锅，两步工艺实现了ADA产率91.4 % 2-呋喃酸。机理研究表明，5-碘戊酸是羰基化过程中的关键中间体。综上所述，本研究为生物源2-呋喃酸合成ADA提供了一种创新且环保的方法，具有很大的工业应用潜力。

{"title":"Adipic acid synthesis from bio-derived 2-furoic acid by reduction-carbonylation","authors":"Changpo Ma , Tiange Zhao , Xiaoxuan Zhang , Shiyu Shen , Yunpu Wang , Lingzhao Kong , Weiran Yang","doi":"10.1016/j.greenca.2025.02.008","DOIUrl":"10.1016/j.greenca.2025.02.008","url":null,"abstract":"<div><div>Adipic acid (ADA) serves as a crucial monomer for the manufacturing of nylon and polyurethanes. However, current production methods are based on petrochemical feedstocks and pose significant environmental concerns. Consequently, the development of an innovative catalytic system for producing ADA from renewable biomass-derived feedstocks is of significant importance. Herein, we report a novel one-pot, two-step process for the highly efficient synthesis of ADA from the biomass derivative 2-furoic acid <em>via</em> hydrogenative carbonylation. In the first step, 2-furoic acid is selectively reduced to 2-tetrahydrofuroic acid using a Rh catalyst with acetic acid (AcOH) and water (H<sub>2</sub>O) as solvents. Subsequently, within the same catalytic system, the addition of I<sub>2</sub> as a promoter enables the further conversion of 2-tetrahydrofuroic acid to ADA through a highly selective carbonylation reaction under CO and H<sub>2</sub> atmospheres. This one-pot, two-step process achieved an ADA yield of 91.4 % from 2-furoic acid. Mechanistic studies revealed that 5-iodopentanoic acid is the key intermediate in the carbonylation process. In summary, this research introduces an innovative and environmentally friendly approach for synthesizing ADA from biomass-derived 2-furoic acid, offering great potential for industrial application.</div></div>","PeriodicalId":100595,"journal":{"name":"Green Carbon","volume":"3 3","pages":"Pages 270-275"},"PeriodicalIF":0.0,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145128389","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Developments of catalysts for the direct conversion of aqueous ethanol to butadiene 水乙醇直接转化丁二烯催化剂的研究进展

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2024.11.008

Na Liu , Mingkai Wang , Yijun Zhou , Lishu Shao , Lin Zhang , Peng Zhan , Zhiping Wu

1,3-Butadiene is an important chemical raw material, especially with its large market demand as the main monomer for rubber tires. It is mainly produced by the thermal cracking of naphtha as a by-product of olefin production. The production process faces dual pressures of petroleum resource consumption and environmental issues. Ethanol, a renewable resource, offers a strategy for green, low-carbon, economical, and sustainable production of butadiene under the "dual carbon" context. This review summarizes the reaction mechanisms, catalyst types, recent research progress, and existing challenges related to the direct conversion of ethanol to butadiene (ETB). It focuses specifically on how water affects catalysts during the direct conversion of aqueous ethanol to butadiene (AETB), offering fresh perspectives and methods for creating effective and hydrophobic catalysts.

1,3-丁二烯是重要的化工原料，尤其作为橡胶轮胎的主要单体，市场需求量大。它主要是由石脑油作为烯烃生产的副产物热裂解产生的。生产过程面临着石油资源消耗和环境问题的双重压力。乙醇作为一种可再生资源，为“双碳”环境下的绿色、低碳、经济、可持续的丁二烯生产提供了策略。本文综述了乙醇直接转化丁二烯（ETB）的反应机理、催化剂类型、最新研究进展以及存在的挑战。它特别关注水在水乙醇直接转化为丁二烯（AETB）过程中如何影响催化剂，为创造有效的疏水催化剂提供了新的视角和方法。

引用次数: 0

Perspective: Roles of rare earth elements in Bacteria 展望：稀土元素在细菌中的作用

Green Carbon

Pub Date : 2025-09-01 DOI: 10.1016/j.greenca.2025.02.007

Changqing Liu , Xiangbo Yin , Huub J.M. Op den Camp , Tobias J. Erb

Rare earth elements (REEs), particularly those within the lanthanide series, have become known to be crucial for microbial methane and methanol oxidation, a key process in the global carbon cycle. This article explores the multifaceted role of REEs, focusing on lanthanide-dependent enzymes, the mechanisms of bacterial uptake of lanthanides, and emerging research areas in respect to the role of lanthanides in bacterial physiology. Despite their name, REEs are relatively abundant in the Earth's crust, and their biological significance is increasingly coming to light, marking a new frontier at the intersection of microbiology and biochemistry.

稀土元素，特别是镧系元素，对于微生物甲烷和甲醇氧化至关重要，这是全球碳循环的一个关键过程。本文探讨了稀土元素的多方面作用，重点关注镧系依赖酶，细菌吸收镧系元素的机制，以及镧系元素在细菌生理中的作用的新兴研究领域。尽管被称为稀土元素，但稀土元素在地壳中相对丰富，其生物学意义日益被人们所认识，标志着微生物学和生物化学交叉领域的一个新前沿。

引用次数: 0

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