Green Chemical Engineering最新文献

英文中文

Poisoning mechanism of Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01 hydrogen storage alloy by trace H2S, CO, and CH4 微量H2S、CO和CH4对Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01储氢合金中毒机理的影响

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-05-09 DOI: 10.1016/j.gce.2025.05.001

Tianmeng He , Xiaoyi Xue , Ke Wang , Honghua Zhang , Ao Li , Yajie Zhang , He Zhang , Hao Wang , Yanrong Liu

TiMn₂-based alloys hold significant application potential due to their moderate hydrogen storage operating conditions and exceptional volumetric hydrogen storage density. Industrial by-product hydrogen, which is widely available and relatively cheap, often contains components such as H₂S, CO, and CH₄, whose poisoning mechanism on TiMn₂-based alloys in the process of hydrogen absorption and desorption remains to be elucidated. In this work, the poisoning mechanisms of H₂S, CO, and CH₄ on Ti_0.8Zr_0.2Cr_0.75Mn_1.25Ce_0.01 hydrogen storage alloy were investigated by isothermal adsorption curve, X-ray photoelectron spectroscopy (XPS), and scanning electron microscope-energy dispersive spectroscopy (SEM-EDS). The results showed that the toxicity of impurity gases on the alloy is CO > H₂S > CH₄, and the regeneration difficulty was H₂S > CO > CH₄. The hydrogen absorption of the Ti_0.8Zr_0.2Cr_0.75Mn_1.25Ce_0.0₁ alloy was restored to 58.59% after five groups of H₂S poisoning-regeneration cycles. The hydrogen storage capacity retention rate decreased to 4.03% after five groups of CO poisoning, but the alloy recovered to 96.62% of the hydrogen absorption capacity after regeneration with pure hydrogen. The retention rate of the alloy was 100% after 100 cycles of CH₄ poisoning. According to the results of XPS analysis, two metal sulfides (TiS and ZrS₂) and one metal sulfate Zr(SO₄)₂ were formed after the Ti_0.8Zr_0.2Cr_0.75Mn_1.25Ce_0.0₁ alloy was poisoned by H₂S. Therefore, H₂S poisoning belongs to irreversible adsorption and CO belongs to reversible adsorption. The poisoning mechanism may guide the design of alloys for the absorption/desorption of industrial by-product hydrogen.

timn2基合金由于其适度的储氢操作条件和卓越的体积储氢密度而具有重要的应用潜力。工业副产氢广泛存在且价格相对低廉，通常含有H2S、CO、CH4等成分，其在吸氢和解吸氢过程中对timn2基合金的中毒机理尚不清楚。采用等温吸附曲线、x射线光电子能谱（XPS）、扫描电镜-能谱（SEM-EDS）研究了H2S、CO和CH4对Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01储氢合金的中毒机理。结果表明：杂质气体对合金的毒性为CO >； H2S > CH4，再生难度为H2S >； CO > CH4；经过5组H2S毒再生循环后，Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01合金的吸氢率恢复到58.59%。5组CO中毒后，储氢容量保留率降至4.03%，但经纯氢再生后，合金的吸氢容量恢复到96.62%。CH4中毒100次后，合金的保留率为100%。XPS分析结果表明，Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01合金受H2S毒害后，形成了两种金属硫化物（TiS和ZrS2）和一种金属硫化物Zr(SO4)2。因此，H2S中毒属于不可逆吸附，CO中毒属于可逆吸附。中毒机理可以指导工业副产氢吸附/解吸合金的设计。

{"title":"Poisoning mechanism of Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01 hydrogen storage alloy by trace H2S, CO, and CH4","authors":"Tianmeng He , Xiaoyi Xue , Ke Wang , Honghua Zhang , Ao Li , Yajie Zhang , He Zhang , Hao Wang , Yanrong Liu","doi":"10.1016/j.gce.2025.05.001","DOIUrl":"10.1016/j.gce.2025.05.001","url":null,"abstract":"<div><div>TiMn2-based alloys hold significant application potential due to their moderate hydrogen storage operating conditions and exceptional volumetric hydrogen storage density. Industrial by-product hydrogen, which is widely available and relatively cheap, often contains components such as H2S, CO, and CH4, whose poisoning mechanism on TiMn2-based alloys in the process of hydrogen absorption and desorption remains to be elucidated. In this work, the poisoning mechanisms of H2S, CO, and CH4 on Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01 hydrogen storage alloy were investigated by isothermal adsorption curve, X-ray photoelectron spectroscopy (XPS), and scanning electron microscope-energy dispersive spectroscopy (SEM-EDS). The results showed that the toxicity of impurity gases on the alloy is CO > H2S > CH4, and the regeneration difficulty was H2S > CO > CH4. The hydrogen absorption of the Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01 alloy was restored to 58.59% after five groups of H2S poisoning-regeneration cycles. The hydrogen storage capacity retention rate decreased to 4.03% after five groups of CO poisoning, but the alloy recovered to 96.62% of the hydrogen absorption capacity after regeneration with pure hydrogen. The retention rate of the alloy was 100% after 100 cycles of CH4 poisoning. According to the results of XPS analysis, two metal sulfides (TiS and ZrS2) and one metal sulfate Zr(SO4)2 were formed after the Ti0.8Zr0.2Cr0.75Mn1.25Ce0.01 alloy was poisoned by H2S. Therefore, H2S poisoning belongs to irreversible adsorption and CO belongs to reversible adsorption. The poisoning mechanism may guide the design of alloys for the absorption/desorption of industrial by-product hydrogen.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"6 4","pages":"Pages 538-550"},"PeriodicalIF":7.6,"publicationDate":"2025-05-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144917732","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

Single solvent synthesis of lithium-selective hydrogen manganese oxide (HMO)-based mixed matrix membranes 单溶剂合成锂选择性氢锰氧化物（HMO）基混合基质膜

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-03-29 DOI: 10.1016/j.gce.2025.03.005

Hafiz M. Saif , Amanuel G. Gebretatios , Rosa M. Huertas , Joao G. Crespo , Sylwin Pawlowski

The rising lithium-ion battery market drives lithium demand and requires efficient and selective lithium recovery methods from aqueous sources. Membrane technologies can address environmental and inherent efficiency issues in conventional lithium extraction methods. This study presents the synthesis of novel lithium-selective mixed matrix membranes (MMMs) by integrating 0–30 wt% of a lithium selective filler named hydrogen manganese oxide (HMO) into a sulfonated polyethersulfone (SPES)-Nafion polymer matrix. The membranes were produced by casting and thoroughly examined to assess their chemical, physical, morphological, thermal, and mechanical characteristics. The transport of lithium across membranes was evaluated in diffusion and electro-diffusion studies. The membrane containing 20 wt% of HMO exhibited the highest ideal selectivity values, which were 1.05 for Li⁺/K⁺, 1.20 for Li⁺/Na⁺, and 13.36 for Li⁺/Mg²⁺; and more than 97% increase in lithium-ion conductivity when compared with the control membrane without HMO. In diffusion experiments, the binary separation factors for Li⁺/K⁺, Li⁺/Na⁺, and Li⁺/Mg²⁺ were 0.71, 1.52, and 11.83, respectively, while under electro-diffusion conditions, the corresponding values were 0.82, 1.55, and 9.88. Above 20 wt% of HMO, membranes lose their separation capacity as HMO aggregates inside the membrane structure. The higher selectivity of membranes towards Li⁺ in the presence of Mg²⁺ is due to magnesium's larger hydrated radius and higher hydration energy compared to lithium. Overall, the prepared membranes demonstrated a promising potential for green lithium recovery. This study facilitates the advancement of sustainable lithium-selective MMM synthesis.

不断增长的锂离子电池市场推动了锂的需求，并要求从水源中高效、选择性地回收锂。膜技术可以解决传统锂提取方法的环境和固有效率问题。本研究提出了一种新型锂选择性混合基质膜（MMMs）的合成方法，将0-30 wt%的锂选择性填料称为氢锰氧化物（HMO）整合到磺化聚醚砜(spe)-Nafion聚合物基体中。这些膜是通过铸造生产的，并进行了彻底的检查，以评估它们的化学、物理、形态、热和机械特性。锂的跨膜运输在扩散和电扩散研究中进行了评估。含20 wt% HMO的膜对Li+/K+、Li+/Na+和Li+/Mg2+的理想选择性值分别为1.05、1.20和13.36；与未添加HMO的对照膜相比，锂离子电导率提高了97%以上。扩散条件下，Li+/K+、Li+/Na+和Li+/Mg2+的二元分离系数分别为0.71、1.52和11.83，电扩散条件下分别为0.82、1.55和9.88。超过20%的HMO，由于HMO聚集在膜结构内，膜失去了分离能力。在Mg2+存在的情况下，膜对Li+有更高的选择性是由于镁的水合半径比锂大，水合能也比锂高。总的来说，所制备的膜显示出绿色锂回收的良好潜力。该研究促进了可持续锂选择性MMM合成的发展。

{"title":"Single solvent synthesis of lithium-selective hydrogen manganese oxide (HMO)-based mixed matrix membranes","authors":"Hafiz M. Saif , Amanuel G. Gebretatios , Rosa M. Huertas , Joao G. Crespo , Sylwin Pawlowski","doi":"10.1016/j.gce.2025.03.005","DOIUrl":"10.1016/j.gce.2025.03.005","url":null,"abstract":"<div><div>The rising lithium-ion battery market drives lithium demand and requires efficient and selective lithium recovery methods from aqueous sources. Membrane technologies can address environmental and inherent efficiency issues in conventional lithium extraction methods. This study presents the synthesis of novel lithium-selective mixed matrix membranes (MMMs) by integrating 0–30 wt% of a lithium selective filler named hydrogen manganese oxide (HMO) into a sulfonated polyethersulfone (SPES)-Nafion polymer matrix. The membranes were produced by casting and thoroughly examined to assess their chemical, physical, morphological, thermal, and mechanical characteristics. The transport of lithium across membranes was evaluated in diffusion and electro-diffusion studies. The membrane containing 20 wt% of HMO exhibited the highest ideal selectivity values, which were 1.05 for Li+/K+, 1.20 for Li+/Na+, and 13.36 for Li+/Mg2+; and more than 97% increase in lithium-ion conductivity when compared with the control membrane without HMO. In diffusion experiments, the binary separation factors for Li+/K+, Li+/Na+, and Li+/Mg2+ were 0.71, 1.52, and 11.83, respectively, while under electro-diffusion conditions, the corresponding values were 0.82, 1.55, and 9.88. Above 20 wt% of HMO, membranes lose their separation capacity as HMO aggregates inside the membrane structure. The higher selectivity of membranes towards Li+ in the presence of Mg2+ is due to magnesium's larger hydrated radius and higher hydration energy compared to lithium. Overall, the prepared membranes demonstrated a promising potential for green lithium recovery. This study facilitates the advancement of sustainable lithium-selective MMM synthesis.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 225-233"},"PeriodicalIF":7.6,"publicationDate":"2025-03-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814418","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

OFC: Outside Front Cover OFC：外封面

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-03-10 DOI: 10.1016/S2666-9528(25)00006-8

引用次数: 0

Outside Back Cover 外封底

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-03-10 DOI: 10.1016/S2666-9528(25)00015-9

引用次数: 0

Sublimation crystallization: from mechanism to applications 升华结晶：从机理到应用

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-02-21 DOI: 10.1016/j.gce.2025.02.001

Sai Wang , Yuntian Xiao , Yitian Su , Yongkang Liu , Shanshan Feng , Hongchen Cao , Ling Zhou , Qiuxiang Yin

Sublimation crystallization, a solvent-free purification technique, has emerged as a sustainable strategy in materials science for producing high-purity substances and advanced functional materials. This review delves into the thermodynamic and kinetic principles governing sublimation crystallization, such as vapor pressure, temperature, and molecular interactions, which play crucial roles in phase transitions and crystal growth. We then explore its practical applications in the separation and purification of materials, the preparation of high-quality single crystals, polymorph and cocrystal screening, and the fabrication of thin films and semiconductor devices. By clarifying the processes and mechanisms involved, this review aims to provide insights into how sublimation crystallization optimizes separation and purification techniques while enhancing material properties as a secondary benefit. This work also outlines future directions and challenges for refining high-efficiency purification methods and advancing sustainable chemical engineering technologies.

升华结晶是一种无溶剂的纯化技术，已成为材料科学领域生产高纯度物质和先进功能材料的可持续发展战略。本文综述了控制升华结晶的热力学和动力学原理，如蒸汽压、温度和分子相互作用，它们在相变和晶体生长中起着至关重要的作用。然后探讨其在材料的分离和纯化、高质量单晶的制备、多晶和共晶筛选、薄膜和半导体器件的制造等方面的实际应用。通过阐明所涉及的过程和机制，本文旨在深入了解升华结晶如何优化分离和纯化技术，同时提高材料性能作为次要优势。本工作还概述了提炼高效净化方法和推进可持续化学工程技术的未来方向和挑战。

{"title":"Sublimation crystallization: from mechanism to applications","authors":"Sai Wang , Yuntian Xiao , Yitian Su , Yongkang Liu , Shanshan Feng , Hongchen Cao , Ling Zhou , Qiuxiang Yin","doi":"10.1016/j.gce.2025.02.001","DOIUrl":"10.1016/j.gce.2025.02.001","url":null,"abstract":"<div><div>Sublimation crystallization, a solvent-free purification technique, has emerged as a sustainable strategy in materials science for producing high-purity substances and advanced functional materials. This review delves into the thermodynamic and kinetic principles governing sublimation crystallization, such as vapor pressure, temperature, and molecular interactions, which play crucial roles in phase transitions and crystal growth. We then explore its practical applications in the separation and purification of materials, the preparation of high-quality single crystals, polymorph and cocrystal screening, and the fabrication of thin films and semiconductor devices. By clarifying the processes and mechanisms involved, this review aims to provide insights into how sublimation crystallization optimizes separation and purification techniques while enhancing material properties as a secondary benefit. This work also outlines future directions and challenges for refining high-efficiency purification methods and advancing sustainable chemical engineering technologies.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 147-167"},"PeriodicalIF":7.6,"publicationDate":"2025-02-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814410","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

Critical evaluation of feature importance assessment in FFNN-based models for predicting Kamlet-Taft parameters 基于ffnn的Kamlet-Taft参数预测模型中特征重要性评估的关键评价

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-01-10 DOI: 10.1016/j.gce.2025.01.003

Yoshiyasu Takefuji

Mohan et al. developed a feed-forward neural network (FFNN) model to predict Kamlet-Taft parameters using quantum chemically derived features, achieving notable predictive accuracy. However, this study raises concerns about conflating prediction accuracy with feature importance accuracy, as high R² and low root mean square error (RMSE) do not guarantee valid feature importance assessments. The reliance on SHapley Additive exPlanations (SHAP) for feature evaluation is problematic due to model-specific biases that could misrepresent true associations. A broader understanding of data distribution, statistical relationships, and significance testing through p-values is essential to rectify this. This paper advocates for employing robust statistical methods, like Spearman's correlation, to effectively assess genuine associations and mitigate biases in feature importance analysis.

Mohan等人开发了一种前馈神经网络（FFNN）模型，利用量子化学衍生的特征来预测Kamlet-Taft参数，取得了显著的预测精度。然而，本研究提出了将预测准确性与特征重要性准确性混为一谈的问题，因为高R2和低均方根误差（RMSE）并不能保证有效的特征重要性评估。依赖SHapley加性解释（SHAP）进行特征评估是有问题的，因为模型特定的偏差可能会歪曲真实的关联。对数据分布、统计关系和通过p值进行显著性检验的更广泛理解对于纠正这一点至关重要。本文提倡采用稳健的统计方法，如斯皮尔曼相关，以有效地评估真正的关联，并减轻特征重要性分析中的偏差。

引用次数: 0

Engineering nano-trap distribution in metal-organic frameworks enables boost of SF6/N2 separation 工程纳米陷阱分布在金属有机框架可以促进SF6/N2分离

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-01-10 DOI: 10.1016/j.gce.2025.01.004

Yan-Long Zhao, Yabo Xie, Xin Zhang, Xiang-Yu Li, Xuefeng Bai, Jian-Rong Li

Separating/capturing SF₆, having the strongest global warming potential, from exhaust gas with low concentration (1%–10%) in the power industry is significant for both greenhouse gas emission control and SF₆ recycling and reutilization. In this study, we achieved highly efficient SF₆/N₂ separation under different SF₆ concentrations (1% and 10%) using two homologous metal-organic frameworks, Ni-bpz and Zn-bpz. This outcome underscores the effectiveness of rational nano-traps distribution engineering for targeted separation applications. The molecular simulation suggests that an SF₆ molecule interacts with a single nano-trap in Zn-bpz. At the same time, it is efficiently confined by two adjacent nano-traps in the parallel distribution of Ni-bpz. Consequently, exceptional SF₆/N₂ selectivity for 1/99 and 10/90 mixtures have been respectively achieved in Ni-bpz (516, SF₆/N₂ = 1/99) and Zn-bpz (608, SF₆/N₂ = 10/90) at 298 K and 1 bar. In dynamic breakthrough experiments, Ni-bpz exhibits a record pure N₂ (≥ 99.99%) productivity (1496 mL/g) for an SF₆/N₂ (1/99) gas mixture. Moreover, both MOFs demonstrate excellent water resistance across multiple cycles, suggesting their high promise for practical application.

从电力行业低浓度（1%-10%）废气中分离/捕集全球变暖潜势最强的SF6，对于控制温室气体排放和SF6回收再利用都具有重要意义。在本研究中，我们利用Ni-bpz和Zn-bpz两种同源金属有机骨架，在不同SF6浓度（1%和10%）下实现了SF6/N2的高效分离。这一结果强调了合理的纳米捕集器分布工程在定向分离应用中的有效性。分子模拟表明，SF6分子与Zn-bpz中的单个纳米陷阱相互作用。同时，在Ni-bpz的平行分布中，它被两个相邻的纳米陷阱有效地限制。因此，在298 K和1 bar条件下，Ni-bpz （516, SF6/N2 = 1/99）和Zn-bpz （608, SF6/N2 = 10/90）对SF6/N2的选择性分别为1/99和10/90。在动态突破实验中，Ni-bpz在SF6/N2（1/99）气体混合物中表现出创纪录的纯N2（≥99.99%）产率（1496 mL/g）。此外，这两种mof在多次循环中都表现出优异的耐水性，这表明它们具有很高的实际应用前景。

{"title":"Engineering nano-trap distribution in metal-organic frameworks enables boost of SF6/N2 separation","authors":"Yan-Long Zhao, Yabo Xie, Xin Zhang, Xiang-Yu Li, Xuefeng Bai, Jian-Rong Li","doi":"10.1016/j.gce.2025.01.004","DOIUrl":"10.1016/j.gce.2025.01.004","url":null,"abstract":"<div><div>Separating/capturing SF6, having the strongest global warming potential, from exhaust gas with low concentration (1%–10%) in the power industry is significant for both greenhouse gas emission control and SF6 recycling and reutilization. In this study, we achieved highly efficient SF6/N2 separation under different SF6 concentrations (1% and 10%) using two homologous metal-organic frameworks, Ni-bpz and Zn-bpz. This outcome underscores the effectiveness of rational nano-traps distribution engineering for targeted separation applications. The molecular simulation suggests that an SF6 molecule interacts with a single nano-trap in Zn-bpz. At the same time, it is efficiently confined by two adjacent nano-traps in the parallel distribution of Ni-bpz. Consequently, exceptional SF6/N2 selectivity for 1/99 and 10/90 mixtures have been respectively achieved in Ni-bpz (516, SF6/N2 = 1/99) and Zn-bpz (608, SF6/N2 = 10/90) at 298 K and 1 bar. In dynamic breakthrough experiments, Ni-bpz exhibits a record pure N2 (≥ 99.99%) productivity (1496 mL/g) for an SF6/N2 (1/99) gas mixture. Moreover, both MOFs demonstrate excellent water resistance across multiple cycles, suggesting their high promise for practical application.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 131-136"},"PeriodicalIF":7.6,"publicationDate":"2025-01-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814408","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

Artificial intelligence for chemical engineering 化学工程中的人工智能

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2025-01-02 DOI: 10.1016/j.gce.2025.01.001

Zhen Song , Weifeng Shen , Zhiwen Qi , José María Ponce Ortega

引用次数: 0

Ionic liquids with multiple hydrogen bonds as metal-free catalysts for efficient hydrolysis of PET under relatively mild conditions 具有多个氢键的离子液体作为无金属催化剂，在相对温和的条件下高效水解PET

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-12-13 DOI: 10.1016/j.gce.2024.12.001

Zhenyu Zhao , Jiayi Bai , Han Tao , Shenyao Wang , Kaili Wang , Wenjun Lin , Lili Jiang , Haoran Li , Congmin Wang

Due to the strong hydrophobicity of PET, chemical catalysts usually require harsh conditions. Herein, inspired by the catalytic sites of PETase, we reported a metal-free catalyst with both high stability and activity, which could achieve almost complete hydrolysis of PET (≥ 99%) under relatively mild conditions (100 °C, PH ≈ 8). Mechanistic investigations showed that hydrogen bonds played an important role. With the increase of hydrogen bond multiplicity and strength, the reaction barrier decreased gradually. We believe that this work might provide a direction for the development of efficient metal-free catalysts and have great industrial application prospects.

由于PET的强疏水性，化学催化剂通常需要苛刻的条件。本文中，受PETase催化位点的启发，我们报道了一种无金属催化剂，具有高稳定性和高活性，在相对温和的条件下（100°C, PH≈8）可以实现PET的几乎完全水解（≥99%）。机理研究表明，氢键起了重要作用。随着氢键数和强度的增加，反应势垒逐渐减小。本研究为高效无金属催化剂的开发提供了方向，具有广阔的工业应用前景。

引用次数: 0

Advances and challenges in N2O valorization for alkane oxidative dehydrogenation to olefins 烷烃氧化脱氢制烯烃N2O气化研究进展与挑战

IF 7.6 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-11-28 DOI: 10.1016/j.gce.2024.11.005

Yunshuo Wu , Xuanhao Wu , Haiqiang Wang , Zhongbiao Wu

Valorization of nitrous oxide (N₂O), a potent greenhouse gas, through the oxidative dehydrogenation of light alkanes such as methane and propane to produce light olefins (ethylene and propylene), presents a promising technique for both environmental mitigation and valuable chemical production. This review provides a systematic analysis of the differences between N₂O and O₂ as oxidants, emphasizing the distinctive advantages of N₂O as a mild oxidant for olefin production. It delves into key technologies, such as oxidative dehydrogenation of propane (ODHP) to propylene and oxidative coupling of methane (OCM) to ethylene, focusing on the underlying reaction mechanisms and recent advancements in catalyst development. A major challenge in these reactions is the trade-off between activity and selectivity. To address this, we propose an innovative strategy–redox center separation–to enhance catalytic performance. This comprehensive review offers valuable insights for the rational design of catalysts, advancing sustainable chemical engineering processes that utilize N₂O, while addressing critical environmental and industrial challenges.

氧化亚氮（N2O）是一种强效温室气体，通过甲烷和丙烷等轻烷烃的氧化脱氢生产轻烯烃（乙烯和丙烯），是一种很有前途的技术，既可以缓解环境，又可以生产有价值的化学品。本文系统分析了氧化亚氮和氧化亚氮作为氧化剂的区别，强调了氧化亚氮作为一种温和氧化剂在烯烃生产中的独特优势。重点介绍了丙烷氧化脱氢制丙烯和甲烷氧化偶联制乙烯等关键技术，重点介绍了反应机理和催化剂的最新进展。这些反应的一个主要挑战是在活性和选择性之间进行权衡。为了解决这个问题，我们提出了一种创新的策略-氧化还原中心分离-以提高催化性能。这一综合综述为合理设计催化剂、推进利用N2O的可持续化学工程过程，同时解决关键的环境和工业挑战提供了有价值的见解。

{"title":"Advances and challenges in N2O valorization for alkane oxidative dehydrogenation to olefins","authors":"Yunshuo Wu , Xuanhao Wu , Haiqiang Wang , Zhongbiao Wu","doi":"10.1016/j.gce.2024.11.005","DOIUrl":"10.1016/j.gce.2024.11.005","url":null,"abstract":"<div><div>Valorization of nitrous oxide (N2O), a potent greenhouse gas, through the oxidative dehydrogenation of light alkanes such as methane and propane to produce light olefins (ethylene and propylene), presents a promising technique for both environmental mitigation and valuable chemical production. This review provides a systematic analysis of the differences between N2O and O2 as oxidants, emphasizing the distinctive advantages of N2O as a mild oxidant for olefin production. It delves into key technologies, such as oxidative dehydrogenation of propane (ODHP) to propylene and oxidative coupling of methane (OCM) to ethylene, focusing on the underlying reaction mechanisms and recent advancements in catalyst development. A major challenge in these reactions is the trade-off between activity and selectivity. To address this, we propose an innovative strategy–redox center separation–to enhance catalytic performance. This comprehensive review offers valuable insights for the rational design of catalysts, advancing sustainable chemical engineering processes that utilize N2O, while addressing critical environmental and industrial challenges.</div></div>","PeriodicalId":66474,"journal":{"name":"Green Chemical Engineering","volume":"7 2","pages":"Pages 137-146"},"PeriodicalIF":7.6,"publicationDate":"2024-11-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145814409","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

首页上一页

下一页尾页

类型

全部化学•材料生命科学医学物理工程技术环境•农林材料科学地球科学法学管理学化学环境科学与生态学计算机科学教育学经济学农林科学人文科学生物学数学物理与天体物理心理学综合性期刊其他工业工程理学历史学农学文学信息工程

数据库

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

期刊

Green Chemical Engineering

全部 Acc. Chem. Res. ACS Applied Bio Materials ACS Appl. Electron. Mater. ACS Appl. Energy Mater. ACS Appl. Mater. Interfaces ACS Appl. Nano Mater. ACS Appl. Polym. Mater. ACS BIOMATER-SCI ENG ACS Catal. ACS Cent. Sci. ACS Chem. Biol. ACS Chemical Health & Safety ACS Chem. Neurosci. ACS Comb. Sci. ACS Earth Space Chem. ACS Energy Lett. ACS Infect. Dis. ACS Macro Lett. ACS Mater. Lett. ACS Med. Chem. Lett. ACS Nano ACS Omega ACS Photonics ACS Sens. ACS Sustainable Chem. Eng. ACS Synth. Biol. Anal. Chem. BIOCHEMISTRY-US Bioconjugate Chem. BIOMACROMOLECULES Chem. Res. Toxicol. Chem. Rev. Chem. Mater. CRYST GROWTH DES ENERG FUEL Environ. Sci. Technol. Environ. Sci. Technol. Lett. Eur. J. Inorg. Chem. IND ENG CHEM RES Inorg. Chem. J. Agric. Food. Chem. J. Chem. Eng. Data J. Chem. Educ. J. Chem. Inf. Model. J. Chem. Theory Comput. J. Med. Chem. J. Nat. Prod. J PROTEOME RES J. Am. Chem. Soc. LANGMUIR MACROMOLECULES Mol. Pharmaceutics Nano Lett. Org. Lett. ORG PROCESS RES DEV ORGANOMETALLICS J. Org. Chem. J. Phys. Chem. J. Phys. Chem. A J. Phys. Chem. B J. Phys. Chem. C J. Phys. Chem. Lett. Analyst Anal. Methods Biomater. Sci. Catal. Sci. Technol. Chem. Commun. Chem. Soc. Rev. CHEM EDUC RES PRACT CRYSTENGCOMM Dalton Trans. Energy Environ. Sci. ENVIRON SCI-NANO ENVIRON SCI-PROC IMP ENVIRON SCI-WAT RES Faraday Discuss. Food Funct. Green Chem. Inorg. Chem. Front. Integr. Biol. J. Anal. At. Spectrom. J. Mater. Chem. A J. Mater. Chem. B J. Mater. Chem. C Lab Chip Mater. Chem. Front. Mater. Horiz. MEDCHEMCOMM Metallomics Mol. Biosyst. Mol. Syst. Des. Eng. Nanoscale Nanoscale Horiz. Nat. Prod. Rep. New J. Chem. Org. Biomol. Chem. Org. Chem. Front. PHOTOCH PHOTOBIO SCI PCCP Polym. Chem.

﹀