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Efficient and scalable upcycling of oceanic carbon sources into bioplastic monomers 有效和可扩展的海洋碳源升级回收到生物塑料单体
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-10-06 DOI: 10.1038/s41929-025-01416-4
Chengbo Li, Mingming Guo, Bo Yang, Yuan Ji, Jing Zhang, Liujiang Zhou, Chunxiao Liu, Haoyuan Wang, Jiawei Li, Weiqing Xue, Xinyan Zhang, Hongliang Zeng, Yanjiang Wang, Donghao Zhao, Kexin Zhong, Shanshan Pi, Minzhe Hei, Xu Li, Qiu Jiang, Tingting Zheng, Xiang Gao, Chuan Xia
Renewable electricity-driven capture and conversion of oceanic dissolved inorganic carbon into value-added chemicals offers a sustainable route towards negative carbon emissions and a circular carbon economy. Here we present an artificial ocean carbon recycling system that captures and converts oceanic carbon sources into biochemicals through a decoupled electro-biocatalytic hybrid process. The system captures CO2 from natural seawater under very dilute yet realistic dissolved inorganic carbon conditions (2.16 mM) with high capture efficiency (>70%), low energy consumption (3 kWh kgCO2−1) and long stability (536 h). Techno-economic analysis revealed a competitive cost of capture (US$229.9 tCO2−1). Using a highly efficient and stable bismuth-based electrocatalyst, CO2 was further converted into pure formic acid (800 mA cm−2 at −1.37 V) and subsequently transformed by engineered Vibrio natriegens into succinic acid (1.37 g l−1). Therefore, our electro-bioconversion system represents a solution to sustainable biochemical synthesis using the ocean carbon sink as a resource. Tandem electro-biocatalytic systems present a versatile platform for producing a variety of synthetic products using CO2 as a starting material. Here direct ocean carbon capture is incorporated into an electrolysis scheme to produce formic acid from CO2 dissolved in seawater that is subsequently converted to succinate in a bioreactor.
可再生电力驱动的海洋溶解无机碳的捕获和转化为增值化学品,为实现负碳排放和循环碳经济提供了一条可持续的途径。在这里,我们提出了一个人工海洋碳回收系统,该系统通过解耦的电-生物催化混合过程捕获海洋碳源并将其转化为生物化学物质。该系统在非常稀释的自然海水中捕获二氧化碳,但实际的溶解无机碳条件(2.16 mM)具有高捕获效率(>70%),低能耗(3 kWh kgCO2−1)和长稳定性(536小时)。技术经济分析显示,捕集具有竞争力的成本(229.9吨二氧化碳−1美元)。利用高效稳定的铋基电催化剂,将CO2进一步转化为纯甲酸(800 mA cm - 2,电压为- 1.37 V),然后通过工程弧菌将其转化为琥珀酸(1.37 g l - 1)。因此,我们的电-生物转换系统代表了利用海洋碳汇作为资源的可持续生化合成的解决方案。串联电-生物催化系统提供了一个通用的平台,用于生产各种合成产品,使用二氧化碳作为起始材料。在这里,直接的海洋碳捕获被纳入电解方案,从溶解在海水中的二氧化碳中产生甲酸,随后在生物反应器中转化为琥珀酸盐。
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引用次数: 0
Predictive model for the discovery of sinter-resistant supports for metallic nanoparticle catalysts by interpretable machine learning 通过可解释的机器学习发现金属纳米颗粒催化剂抗烧结支撑的预测模型
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-29 DOI: 10.1038/s41929-025-01417-3
Chenggong Jiang, Bill Yan, Bryan R. Goldsmith, Suljo Linic
The metal–support interaction (MSI) critically influences the performance of supported nanocatalysts and their long-term stability, yet the factors governing MSIs are multifaceted and challenging to sort out. Here we combine first-principles neural network molecular dynamics (NN-MD) simulations with interpretable machine learning (iML) to shed light on the factors determining MSIs for Pt nanoparticles on diverse metal–oxide supports. Our approach reveals the atomic-scale dynamics of sintering mechanisms and identifies key features of oxide supports governing MSI. We find that the surface energy, surface oxygen bond order, surface dipole and work function of the support are dominant in Pt–oxide interactions. Leveraging these insights, we screened promising sinter-resistant supports for Pt nanoparticles from over 10,000 metal–oxide surfaces and validated some cases by Monte Carlo simulations and experiments. This work integrates iML with NN-MD to accelerate the understanding and discovery of stable supported nanocatalysts, and should be broadly applicable to numerous catalytic applications. The activity and stability of supported metal catalysts is in large part influenced by their interaction with the support. Now, neural network molecular dynamics simulations are combined with interpretable machine learning to reveal the governing factors of metal–support interactions for Pt nanoparticles on various oxide supports, identifying key features and proposing sinter-resistant supports.
金属-载体相互作用(MSI)对负载型纳米催化剂的性能及其长期稳定性有重要影响,但影响MSI的因素是多方面的,难以理清。在这里,我们将第一性原理神经网络分子动力学(NN-MD)模拟与可解释机器学习(iML)相结合,揭示了决定不同金属氧化物载体上Pt纳米颗粒msi的因素。我们的方法揭示了烧结机制的原子尺度动力学,并确定了氧化物支撑体控制MSI的关键特征。我们发现表面能、表面氧键顺序、表面偶极子和载体的功函数在pt -氧化物相互作用中占主导地位。利用这些见解,我们从超过10,000种金属氧化物表面筛选了有希望的Pt纳米颗粒抗烧结支撑,并通过蒙特卡罗模拟和实验验证了一些情况。这项工作将iML与NN-MD相结合,以加速对稳定负载纳米催化剂的理解和发现,并应广泛适用于许多催化应用。负载型金属催化剂的活性和稳定性在很大程度上受其与载体相互作用的影响。现在,神经网络分子动力学模拟与可解释的机器学习相结合,揭示了Pt纳米颗粒在各种氧化物载体上的金属-载体相互作用的控制因素,确定了关键特征,并提出了抗烧结载体。
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引用次数: 0
The (mis)uses of Tafel slope 塔菲尔斜坡的(错误)使用
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01397-4
Valentin Briega-Martos, Rafael Guzman-Soriano, Jiahong Jiang, Yao Yang
Tafel slope analysis, first proposed by Julius Tafel in 1905 and supported by the Butler–Volmer equation, is widely used to elucidate electrocatalytic mechanisms and evaluate kinetics. However, some misuses still frequently occur in the literature, calling for rigorous mechanistic investigations at single-crystal electrodes and under well defined mass-transport conditions.
Tafel斜率分析由Julius Tafel于1905年首次提出,并得到Butler-Volmer方程的支持,被广泛用于阐明电催化机理和评价动力学。然而,在文献中仍然经常出现一些误用,要求在单晶电极和明确的质量输运条件下进行严格的机制研究。
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引用次数: 0
Oxidative cleavage of hexopyranose by a TIM-barrel isomerase tim桶异构酶氧化裂解己糖
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01412-8
Pengwei Li, Dacheng Wang, Lu Guo, Yanru Chen, Huijin Mao, Zelian Zhao, Min Wang, Meng Chen, Zhengren Xu, Binju Wang, Defeng Li, Yihua Chen
Cleavage of hexopyranose to short-chain carbohydrates plays crucial roles in carbon metabolism and energy supply. Currently, the carbon–carbon bond scission of hexopyranose involves two types of reaction: the widely distributed retro-aldol reaction and the transketo-like reaction observed in Bifidobacteria. Here we report the discovery and characterization of metalloenzyme Art22, which is involved in the sugar moiety modification of aurantinin B (ART B), an antibacterial agent from Bacillus. Art22 adopts a TIM-barrel fold, enabling the activation of 4-keto ART B into potent antibiotic ART B via rapid isomerization. In addition, it protects the ART-producing Bacillus by detoxifying cellular ART B to ART B1–B3 via slow oxidative cleavage of the 3-keto hexopyranose to short-chain carbohydrates and CO2. Guided by structural, mutagenic and computational studies, we reveal an anhydride-mediated mechanism for Art22-catalysed oxygenation reactions, which expands the catalytic repertoire of TIM-barrel enzymes and adds an oxidative path for hexopyranose cleavage. Hexopyranose cleavage is a crucial step in carbon metabolism. Here the authors report the discovery and characterization of metalloenzyme Art22, which is involved in the sugar moiety modification of aurantinin B, an antibacterial agent from Bacillus.
六吡喃糖裂解成短链碳水化合物在碳代谢和能量供应中起着至关重要的作用。目前己吡喃糖的碳-碳键断裂涉及两种反应:广泛分布的反醛醇反应和双歧杆菌中观察到的类转酮反应。本文报道了一种新的金属酶Art22的发现和鉴定,该酶参与了来自芽孢杆菌的一种抗菌剂金菌素B (aurantinin B, ART B)的糖段修饰。Art22采用TIM-barrel折叠,通过快速异构化使4-酮类ART B活化为强效抗生素ART B。此外,它通过将3-酮己糖缓慢氧化裂解为短链碳水化合物和二氧化碳,将细胞中的ART B解毒为ART B1-B3,从而保护产生ART的芽胞杆菌。在结构、诱变和计算研究的指导下,我们揭示了一种酸酐介导的art22催化氧化反应机制,这扩大了tim桶酶的催化范围,并增加了六吡喃糖裂解的氧化途径。六吡喃糖的裂解是碳代谢的关键步骤。本文报道了一种新的金属酶Art22的发现和鉴定,该酶参与了金霉素B的糖段修饰。
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引用次数: 0
Pushing the boundaries of biocatalysis 推动生物催化的发展
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01415-5
Rudi Fasan
The 2025 RepArtZymes conference featured the latest developments in the design and development of artificial and repurposed enzymes for synthetic and biotechnological applications. These contributions illustrate the impact of this rapidly expanding research area towards addressing key challenges in organic synthesis, medicinal chemistry, polymer chemistry, energy conversion, and environmental remediation.
2025年RepArtZymes会议重点介绍了用于合成和生物技术应用的人工酶和再利用酶的设计和开发的最新进展。这些贡献说明了这一迅速扩大的研究领域对解决有机合成、药物化学、聚合物化学、能量转化和环境修复等关键挑战的影响。
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引用次数: 0
From isotherms to modern kinetics 从等温线到现代动力学
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01401-x
Dmitry Yu. Murzin
Adsorption on solid surfaces is extremely important for various phenomena and applications. In the 1910s, adsorption and subsequent catalysis was described mainly in terms of diffusion through a fluid film to the interface. Langmuir developed the concept of a monolayer adsorption, which became the cornerstone of modern surface science.
固体表面的吸附对于各种现象和应用都是非常重要的。在20世纪10年代,吸附和随后的催化作用主要是通过流体膜扩散到界面来描述的。朗缪尔提出了单层吸附的概念,成为现代表面科学的基石。
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引用次数: 0
Dynamic and durable 动态持久
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01422-6
Lin Li
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引用次数: 0
Electrolysis in tandem 串联电解
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01424-4
Benjamin Martindale
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引用次数: 0
From descriptive to quantitative biocatalysis 从描述到定量的生物催化
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01400-y
Peter Westh, Jeppe Kari
The 1913 study ‘Die Kinetik der Invertinwirkung’, by Michaelis and Menten, marked a pivotal advancement in enzymology by illustrating the application of mechanistic models and quantitative kinetics to biocatalysis. The foundational framework described back then continues to have a strong impact on enzymology, with profound influences that range from undergraduate education to structure–function studies and the format and content of contemporary kinetic databases.
1913年Michaelis和Menten的研究“Die Kinetik der Invertinwirkung”,通过说明机理模型和定量动力学在生物催化中的应用,标志着酶学的关键进步。当时描述的基本框架继续对酶学产生强烈的影响,从本科教育到结构-功能研究以及当代动力学数据库的格式和内容都产生了深远的影响。
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引用次数: 0
Establishing coupling trends 建立耦合趋势
IF 44.6 1区 化学 Q1 CHEMISTRY, PHYSICAL Pub Date : 2025-09-24 DOI: 10.1038/s41929-025-01423-5
Marçal Capdevila-Cortada
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Nature Catalysis
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