Green Chemistry最新文献

筛选
英文 中文
Transforming volatile amines into stable solid sorbents via crosslinking for direct air capture of carbon dioxide 通过交联将挥发性胺转化为稳定的固体吸附剂,直接捕获空气中的二氧化碳
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-15 DOI: 10.1039/d5gc06981e
Ethan Adam, Zhijian Wan, Arash Arami-Niya, Durga Acharya, Wendy Tian, Colin D. Wood
{"title":"Transforming volatile amines into stable solid sorbents via crosslinking for direct air capture of carbon dioxide","authors":"Ethan Adam,&nbsp;Zhijian Wan,&nbsp;Arash Arami-Niya,&nbsp;Durga Acharya,&nbsp;Wendy Tian,&nbsp;Colin D. Wood","doi":"10.1039/d5gc06981e","DOIUrl":"10.1039/d5gc06981e","url":null,"abstract":"<div><div>Supported amines are popular solid sorbents for direct air capture (DAC) of carbon dioxide (CO<sub>2</sub>). However, those sorbents have several drawbacks such as leaching, volatility, oxidative degradation and corrosivity, among others. In this work, solid crosslinked (CL) polymers without the need of support were synthesised from several short chain amines that would be otherwise unviable for DAC due to their high volatility. This was achieved utilising an epoxide crosslinker <em>N</em>,<em>N</em>,<em>N</em>′,<em>N</em>′-tetrakis(2,3-epoxypropyl)-<em>m</em>-xylene-alpha,alpha′-diamine (TEP-MXDA), and small amines including ethylenediamine (EtDA), diaminobutane (DAB), hexamethylenediamine (HMD), diethylenetriamine (DET), triethylenetetramine (TETA) and <em>m</em>-xylylenediamine (<em>m</em>XDA) through a one-pot procedure at room temperature for 12 hours. The reaction yielded no wastes, no side products and required no separation and purification, adhering to 11 of the 12 principles of green chemistry overall. Under realistic DAC conditions, CO<sub>2</sub> absorption capacities up to 5.6 wt% were achieved for CL-DET polymers. Additionally, the CL-TETA and CL-HMD polymers retained a greater CO<sub>2</sub> capacity compared to their silica supported counterparts after accelerated ageing tests conducted in air at 75 °C for 24 hours, corresponding to approximately 150 absorption/desorption cycles. Novel insight into the effect of amine chain length on resulting polymer mesh size and CO<sub>2</sub> absorption capacity is provided by positron annihilation lifetime spectroscopy (PALS) analysis, and reveals the beneficial role PEG plays in hydrogel-like amine-based crosslinked sorbents. This study demonstrates the viability of crosslinked short-chain amines as solid sorbents for DAC applications, and provides novel insight into the effects variables such as amine choice, amine chain length and crosslinking ratio have on the performance of the resulting materials in CO<sub>2</sub> absorption.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11295-11307"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545627","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
Enhanced lignin hydrogenolysis by in situ hydrogen supply through methanol–water aqueous phase reforming over a CoTi@biochar catalyst 在CoTi@biochar催化剂上通过甲醇-水水相重整原位供氢增强木质素氢解
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-08 DOI: 10.1039/d6gc00372a
Tao Yin, Zhaoyuan Huang, Bowen Luo, Zhipeng Tian, Chao Wang, Jianping Liu, Ying Chen, Riyang Shu
{"title":"Enhanced lignin hydrogenolysis by in situ hydrogen supply through methanol–water aqueous phase reforming over a CoTi@biochar catalyst","authors":"Tao Yin,&nbsp;Zhaoyuan Huang,&nbsp;Bowen Luo,&nbsp;Zhipeng Tian,&nbsp;Chao Wang,&nbsp;Jianping Liu,&nbsp;Ying Chen,&nbsp;Riyang Shu","doi":"10.1039/d6gc00372a","DOIUrl":"10.1039/d6gc00372a","url":null,"abstract":"<div><div>A novel catalytic strategy for enhanced lignin hydrogenolysis by <em>in situ</em> hydrogen supply was developed over a CoTi@biochar catalyst. In this catalytic system, methanol is used as the solvent for lignin hydrogenolysis. The suitable addition of water promotes the methanol–water aqueous phase reforming (APR) reaction for <em>in situ</em> hydrogen supply, which enhances the lignin hydrogenolysis performance. The synergistic interaction between Co and Ti species not only promotes the APR reaction for hydrogen production, but also improves the hydrogenolysis of lignin. The proposed strategy offers a promising approach for advancing lignin valorization and sustainable biorefinery technologies.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 10954-10964"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545654","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
Dual-benefit flash pyrolysis for valorizing carbonaceous wastes into high-calorific syngas (94.7 vol% combustibles) and battery anodes 双效益闪蒸热解将含碳废物转化为高热量合成气(94.7 vol%可燃物)和电池阳极
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-05-21 DOI: 10.1039/d6gc00839a
Pengfei Huang, Li Chen, Zekun Li, Zhedong Liu, Wei-Di Liu, Jingchao Zhang, Jiawei Luo, Wenjun Zhang, Xinxi Zhang, Rongtao Zhu, Yanan Chen
{"title":"Dual-benefit flash pyrolysis for valorizing carbonaceous wastes into high-calorific syngas (94.7 vol% combustibles) and battery anodes","authors":"Pengfei Huang,&nbsp;Li Chen,&nbsp;Zekun Li,&nbsp;Zhedong Liu,&nbsp;Wei-Di Liu,&nbsp;Jingchao Zhang,&nbsp;Jiawei Luo,&nbsp;Wenjun Zhang,&nbsp;Xinxi Zhang,&nbsp;Rongtao Zhu,&nbsp;Yanan Chen","doi":"10.1039/d6gc00839a","DOIUrl":"10.1039/d6gc00839a","url":null,"abstract":"<div><div>Traditional low-temperature slow pyrolysis (LTSP) is inefficient and constrained by low temperatures (300–1000 °C) and prolonged durations, leading to poor kinetics and high energy demand. This work demonstrates an innovative <em>in situ</em> Joule heating technology to achieve ultra-high-temperature flash pyrolysis (UHTFP) at over 3000 °C in approximately one second. This method ensures complete pyrolysis, resulting in enhanced product purity, efficiency, and yield compared with LTSP. The versatility of UHTFP is highlighted by its exceptional product selectivity: the pyrolysis of anthracite yields a hydrogen-rich gas (up to 83.7% H<sub>2</sub>), while bituminous coal is efficiently converted into a premium, high-calorific syngas, with combustible monomers (H<sub>2</sub>, CO, and CH<sub>4</sub>) constituting an impressive 94.7 vol% of the product gas. Molecular dynamics simulations show that the ultra-high-temperature system in a non-equilibrium state can generate numerous free radicals, causing the carbon atoms to be condensed into flash graphene and the heteroatoms to be fragmented into small gas molecules. Moreover, the obtained flash graphene can be used as the negative electrode of lithium-ion batteries, exhibiting a specific capacity of 326.83 mAh g<sup>−1</sup>. The UHTFP technology is versatile, scalable and capable of swiftly processing materials, such as coal, biomass, and waste plastics, offering significant economic and environmental advantages for chemical and energy production.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11096-11106"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545662","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
Deep eutectic solvent-mediated medical dressings: the evolution from green processing solvents to multifunctional integrated media 深共晶溶剂介质医用敷料:从绿色加工溶剂到多功能集成介质的演变
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-10 DOI: 10.1039/d6gc01943a
Zexin Lin, Caiyue Le, Zhixia Li, Dan Kong, Yani Guo, Yimin Sun
{"title":"Deep eutectic solvent-mediated medical dressings: the evolution from green processing solvents to multifunctional integrated media","authors":"Zexin Lin,&nbsp;Caiyue Le,&nbsp;Zhixia Li,&nbsp;Dan Kong,&nbsp;Yani Guo,&nbsp;Yimin Sun","doi":"10.1039/d6gc01943a","DOIUrl":"10.1039/d6gc01943a","url":null,"abstract":"<div><div>Deep eutectic solvents (DESs) represent an emerging class of environmentally friendly solvents formed <em>via</em> the complexation of hydrogen bond donors and acceptors. Owing to their superior solvation capabilities, structural tunability, and intrinsic bioactivity, DESs hold considerable promise for reshaping the development of advanced medical dressings. This review systematically summarizes the technological evolution of DESs from conventional processing solvents to multifunctional integrated media. Furthermore, the versatile applications of DESs are comprehensively discussed, encompassing their roles as functional platforms, structure-directing and dynamic crosslinking agents, drug carriers for controlled release, and electroconductive and sensing elements. Subsequently, the current challenges in processing DES-mediated fiber-based medical dressings are outlined. Additionally, a conceptual design for next-generation smart dressings based on a “dry storage–<em>in situ</em> activation” strategy is proposed, offering new insights to facilitate the clinical translation of high-performance dressings.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 10931-10953"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545653","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
CuMoRu ternary alloy nanorods: synergy effect of metal elements enables efficient electrochemical CO2 reduction towards selective ethanol production CuMoRu三元合金纳米棒:金属元素的协同效应,使电化学二氧化碳减少到选择性乙醇生产
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-04 DOI: 10.1039/d6gc00844e
Dong Xiang, Huanzong Liao, Ziyi Gui, Dezhong Hu, Kunzhen Li, Kanghua Miao, Aidar Kuchkaev, Dmitry G. Yakhvarov, Xiongwu Kang, Xiufang Wang
{"title":"CuMoRu ternary alloy nanorods: synergy effect of metal elements enables efficient electrochemical CO2 reduction towards selective ethanol production","authors":"Dong Xiang,&nbsp;Huanzong Liao,&nbsp;Ziyi Gui,&nbsp;Dezhong Hu,&nbsp;Kunzhen Li,&nbsp;Kanghua Miao,&nbsp;Aidar Kuchkaev,&nbsp;Dmitry G. Yakhvarov,&nbsp;Xiongwu Kang,&nbsp;Xiufang Wang","doi":"10.1039/d6gc00844e","DOIUrl":"10.1039/d6gc00844e","url":null,"abstract":"<div><div>Copper (Cu)-based alloy catalysts are promising for converting CO<sub>2</sub> to hydrocarbons and oxygenated compounds through the electrochemical CO<sub>2</sub> reduction reaction (eCO<sub>2</sub>RR). However, it remains a great challenge to selectively obtain ethanol among the C<sub>2</sub> products from eCO<sub>2</sub>RR. Herein, CuMoRu alloy nanorod catalysts were synthesized by a one-pot wet chemistry method. Compared with Cu, CuRu and CuMo catalysts, CuMoRu is more efficient in converting CO<sub>2</sub> to ethanol in eCO<sub>2</sub>RR. Theoretical calculations illustrate that Mo and Ru doping onto a Cu substrate leads to suppressed hydrogen evolution reaction (HER), enhanced *CO production, and the formation of C<sub>2</sub> products occurs <em>via</em> an asymmetrical *CO–*CHO coupling pathway. Additionally, the stabilization of CH<sub>2</sub>CHO* and enhanced H<sub>2</sub>O dissociation benefit ethanol production by breaking the scaling relationship. In a flow cell, CuMoRu displays a faradaic efficiency of 63.0% and 51.8% for C<sub>2</sub> products and C<sub>2</sub>H<sub>5</sub>OH at −1.1 V <em>vs.</em> the reversible hydrogen electrode (RHE), respectively, and the corresponding total and C<sub>2</sub> partial current density is 290 and 182.7 mA cm<sup>−2</sup> in an alkaline electrolyte, respectively. <em>In situ</em> Raman spectroscopy demonstrated that the CuMoRu interface exhibits increased CO<sub>b</sub> (CO on bridging site) coverage and local pH, and the directly observed vibrational bands from *COCHO confirm the asymmetrical *CO–*CHO coupling mechanism. This work highlights the importance of alloying metal with Cu for the selective production of C<sub>2</sub> products in eCO<sub>2</sub>RR.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11262-11272"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545691","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
Cerium oxide-supported positively charged platinum single atoms enable efficient decalin dehydrogenation under mild conditions 氧化铈负载的带正电铂单原子在温和条件下实现了高效的十氢化萘脱氢
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-16 DOI: 10.1039/d6gc01089j
Dongyang Zhao, Cuncai Lv, Li Li, Linjie Gao, Shangbo Ning, Yuchen Hao, Yanhui Fu, Yaguang Li, Jinhua Ye
{"title":"Cerium oxide-supported positively charged platinum single atoms enable efficient decalin dehydrogenation under mild conditions","authors":"Dongyang Zhao,&nbsp;Cuncai Lv,&nbsp;Li Li,&nbsp;Linjie Gao,&nbsp;Shangbo Ning,&nbsp;Yuchen Hao,&nbsp;Yanhui Fu,&nbsp;Yaguang Li,&nbsp;Jinhua Ye","doi":"10.1039/d6gc01089j","DOIUrl":"10.1039/d6gc01089j","url":null,"abstract":"<div><div>Efficient decalin dehydrogenation is essential for hydrogen (H<sub>2</sub>) release in liquid organic hydrogen carrier (LOHC) systems. However, its strongly endothermic nature necessitates high temperatures, which promote aggregation of platinum (Pt) nanoparticles in conventional catalysts, leading to performance loss and high metal loading requirements. Addressing this challenge, we designed a ceria-supported Pt single-atom catalyst (Pt SAC/CeO<sub>2</sub>) that maximizes atomic utilization and resists sintering through robust metal–support interactions and abundant oxygen vacancies. Integrated spectroscopic analyses and density functional theory (DFT) calculations reveal that these interactions generate positively charged Pt species that lower the activation barrier for the initial C–H bond scission and facilitate desorption of dehydrogenated aromatics, collectively enhancing catalytic efficiency. The optimized Pt SAC/CeO<sub>2</sub> catalyst achieves an exceptional H<sub>2</sub> production rate of 3126 mmol g<sub>Pt</sub><sup>−1</sup> h<sup>−1</sup> at 260 °C in a continuous-flow reactor, surpassing commercial Pt/C catalysts. Furthermore, coupling Pt SAC/CeO<sub>2</sub> with a solar-thermal device enables sunlight-driven decalin dehydrogenation, delivering 3140 mmol g<sub>Pt</sub><sup>−1</sup> h<sup>−1</sup> under 0.5 kW m<sup>−2</sup> and generating 11.6 L of H<sub>2</sub> per day without external power. Our study sheds light on charge modulation strategies for single-atom catalysts and provides a feasible pathway towards practical LOHC dehydrogenation processes.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11308-11315"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545553","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
Ultrasound-generated cyclodextrin–amino acid inclusion complex with NH3+-mediated chalcone activation: metal-free catalysis surpassing nanoparticles 超声波生成的环糊精-氨基酸包合物与NH3+介导的查尔酮活化:超越纳米颗粒的无金属催化
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-10 DOI: 10.1039/d6gc01518b
Divya Tagra, Mamta Guleria, Jyoti Agarwal
{"title":"Ultrasound-generated cyclodextrin–amino acid inclusion complex with NH3+-mediated chalcone activation: metal-free catalysis surpassing nanoparticles","authors":"Divya Tagra,&nbsp;Mamta Guleria,&nbsp;Jyoti Agarwal","doi":"10.1039/d6gc01518b","DOIUrl":"10.1039/d6gc01518b","url":null,"abstract":"<div><div>Efficient cycloaddition of chalcones remains challenging due to extensive π-delocalization and steric shielding of the α,β-unsaturated carbonyl unit, which limit classical Lewis-acid activation strategies. Here, we report a metal-free supramolecular organocatalytic platform that enables selective chalcone activation through noncovalent Lewis-acidic interactions. The catalyst comprises NH<sub>3</sub><sup>+</sup>-bearing amino acids embedded within cyclodextrin inclusion complexes, assembled <em>via</em> ultrasound energy. Mechanistically, directional N–H⋯O hydrogen bonding and localized electrostatic polarization activate the chalcone carbonyl, while cyclodextrin-mediated confinement enforces productive orientation and transition-state stabilization. This compact activation mode overcomes steric constraints imposed by bulky aromatic substituents, delivering cycloaddition reactions with enhanced activity providing the yields up to 97% under mild conditions in ethanol. The system outperforms conventional metal nanoparticle-based catalysts, preserves substrate integrity, and exhibits broad functional-group tolerance. This work establishes a generalizable, sustainable paradigm for chalcone cycloaddition catalysis by synergistically integrating organocatalytic Lewis acidity with supramolecular confinement.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11018-11035"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545605","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
Highly dispersed Mo2C/AC for gas-phase catalytic direct deoxygenation during lignin pyrolysis 木质素热解过程中气相催化直接脱氧的高分散Mo2C/AC
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-12 DOI: 10.1039/d6gc01475e
Jiajun Yu, Wujin Xu, Mingxun Zeng, Kai Wu, Wei Jin, Leilei Dai, Shurong Wang, Huiyan Zhang
{"title":"Highly dispersed Mo2C/AC for gas-phase catalytic direct deoxygenation during lignin pyrolysis","authors":"Jiajun Yu,&nbsp;Wujin Xu,&nbsp;Mingxun Zeng,&nbsp;Kai Wu,&nbsp;Wei Jin,&nbsp;Leilei Dai,&nbsp;Shurong Wang,&nbsp;Huiyan Zhang","doi":"10.1039/d6gc01475e","DOIUrl":"10.1039/d6gc01475e","url":null,"abstract":"<div><div>Lignin pyrolysis can efficiently produce renewable aromatic hydrocarbons, but the selective cleavage of lignin C–O bonds and the inhibition of intermediate polycondensation in solvent-free systems remain significant challenges. This work proposes a strategy coupling gas-phase lignin pyrolysis with online hydrodeoxygenation, employing highly dispersed Mo<sub>2</sub>C to achieve targeted deoxygenation of lignin toward aromatics. Mo<sub>2</sub>C/AC exhibits high direct deoxygenation selectivity over a wide temperature range (300–500 °C), which facilitates selective C–O bond cleavage while inhibiting catalyst coking and aromatic ring cracking. The aromatic hydrocarbon yield from guaiacol reached as high as 93 mol%, with 100% selectivity. Specifically, Mo<sub>2</sub>C effectively mitigates the high-temperature condensation of guaiacol by removing oxygen-containing groups, thereby inhibiting the formation of oligomers. Compared with traditional zeolite-catalysed lignin pyrolysis at the same temperature, the yield of monocyclic aromatic hydrocarbons increased by 344%, while coke formation was reduced to only 20% of the original level. After birch lignin pyrolysis coupled with hydrodeoxygenation, the yield of monomeric aromatic hydrocarbons can reach up to 11.3 wt%. This study achieves selective deoxygenation of lignin in the gas phase at low temperature while significantly suppressing catalyst coking, offering a viable strategy for efficient solvent-free lignin conversion.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11240-11252"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545626","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
Bayesian optimization and molecular dynamics simulations to guide protic ionic liquid-based biorefining for efficient lignin applications 贝叶斯优化和分子动力学模拟指导基于质子离子液体的高效木质素生物精制
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-05 DOI: 10.1039/d6gc02613c
Sharib Khan, Tormi Lillerand, Veerapandian Ponnuchamy, A. G. M. Zaman, Daniel Rauber, Udayakumar Veerabagu, Jüri Olt, Markus Gallei, Sabarathinam Shanmugam, Timo Kikas
{"title":"Bayesian optimization and molecular dynamics simulations to guide protic ionic liquid-based biorefining for efficient lignin applications","authors":"Sharib Khan,&nbsp;Tormi Lillerand,&nbsp;Veerapandian Ponnuchamy,&nbsp;A. G. M. Zaman,&nbsp;Daniel Rauber,&nbsp;Udayakumar Veerabagu,&nbsp;Jüri Olt,&nbsp;Markus Gallei,&nbsp;Sabarathinam Shanmugam,&nbsp;Timo Kikas","doi":"10.1039/d6gc02613c","DOIUrl":"10.1039/d6gc02613c","url":null,"abstract":"<div><div>The transition to a circular bioeconomy depends on the sustainable use of renewable resources, with forest-based biomass playing a critical role. Lignin, in particular, is a promising feedstock for replacing fossil-derived aromatics due to its unique chemical structure. However, lignin obtained from conventional pulp mills often contains impurities and structural modifications that limit its potential for producing high-value chemicals and materials. In contrast, emerging biorefinery pretreatment strategies enable a “lignin-focused” approach, where every major biomass component, cellulose, hemicelluloses, and lignin, is valorized for intended applications, allowing the tailored production of bio-based products with improved structural quality. Traditionally, the development of biorefining processes requires extensive experimentation guided largely by empirical advances. In this study, we demonstrate how Bayesian optimization can accelerate the development of a sustainable biomass fractionation process based on the protic ionic liquid (PIL) triethylammonium hydrogen sulfate ([TEA][HSO<sub>4</sub>]). Open-source Python-based tools were employed to optimize lignin extraction from softwood and evaluate the influence of key processing parameters, including temperature and process severity, on lignin yield. Molecular dynamics simulations and in-depth literature analyses were adopted to identify the optimal trade-offs between lignin recovery and structural properties. Notably, the optimized PIL fractionation process achieved 82% delignification with lignin yields of up to 73%, while consistently producing lignin with low molecular weights because of <em>in situ</em> depolymerization during pretreatment. Furthermore, advanced qualitative characterization was conducted to assess the lignin structure and evaluate the relationship between lignin yield, structural quality, and potential downstream applications.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11057-11076"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545660","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
Systematic metabolic engineering combined with iterative SCRaMbLE boosts sweetener thaumatin production by Saccharomyces cerevisiae 系统的代谢工程与迭代的SCRaMbLE相结合,促进了酿酒酵母菌的甜味剂合成
IF 10.6 1区 化学
Green Chemistry Pub Date : 2026-07-06 Epub Date: 2026-06-03 DOI: 10.1039/d6gc01471b
Yani Zhao, Yunpeng Lv, Zhongxin Cui, Yong Zhu, Lei Zhang, Haishan Qi
{"title":"Systematic metabolic engineering combined with iterative SCRaMbLE boosts sweetener thaumatin production by Saccharomyces cerevisiae","authors":"Yani Zhao,&nbsp;Yunpeng Lv,&nbsp;Zhongxin Cui,&nbsp;Yong Zhu,&nbsp;Lei Zhang,&nbsp;Haishan Qi","doi":"10.1039/d6gc01471b","DOIUrl":"10.1039/d6gc01471b","url":null,"abstract":"<div><div>Thaumatin is a natural sweet protein with excellent thermal stability and high commercial value, serving as an ideal sucrose substitute in the food industry. However, its sustainable application has been limited by low natural abundance in plant sources and high extraction costs. Herein, multi-dimensional engineering of <em>Saccharomyces cerevisiae</em> was employed to significantly enhance thaumatin production. First, systematic optimization of the expression system—including the promoter, terminator, and signal peptide—enabled the engineered strain to achieve a titer of 129.3 mg L<sup>−1</sup>. Subsequently systematic metabolic engineering, targeting transcription, translation, secretion, and degradation pathways, increased the titer to 320.0 mg L<sup>−1</sup>. To further break through the productivity bottleneck, genome rearrangement was conducted using a SCRaMbLE system, yielding a high–producing mutant yYPLV-4, which exhibited a 2.96-fold increase over the parental strain. Integrated multi-omics analysis revealed crucial genetic modifications and metabolic reprogramming events, including enhanced amino acid biosynthesis, reduced ubiquitination and byproduct formation. Guided by these insights, combinatorial engineering of high-yield targets further elevated the titer to 467.7 mg L<sup>−1</sup>. Following fermentation optimization, fed-batch fermentation in a 5 L bioreactor yielded a final thaumatin titer of 3.04 g L<sup>−1</sup> – the highest level reported to date. This study establishes a new benchmark for microbial thaumatin production and provides an adaptable framework that integrates systematic engineering with SCRaMbLE-based genome remodeling to build efficient heterologous protein-producing cell factories.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"28 26","pages":"Pages 11077-11095"},"PeriodicalIF":10.6,"publicationDate":"2026-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"148545661","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
0
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
相关产品
×
本文献相关产品
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信
小红书