Green Chemical Engineering最新文献

英文中文

Tailored SrFeO3-δ for chemical looping dry reforming of methane 用于甲烷化学循环干式转化的定制 SrFeO3-δ

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-04-23 DOI: 10.1016/j.gce.2024.04.003

Ao Zhu, Dongfang Li, Tao Zhu, Xing Zhu

Chemical looping dry reforming of methane (CL-DRM) is a highly efficient process that converts two major greenhouse gases (CH₄ and CO₂) into syngas ready for the feedstock of liquid fuel production. One of the major obstacles facing this technology now is creating oxygen carriers that are stable and reactive. We fabricated high-performance Sr_0.98Fe_0.7Co_0.3O_3-δ perovskite-structured oxygen carrier by combining A-site defects and B-site doping of SrFeO_3-δ. During isothermal CL-DRM tests at 850 °C, Sr_0.98Fe_0.7Co_0.3O_3-δ achieved 87% CH₄ conversion and 94% CO selectivity in the CH₄ partial oxidation reaction, followed by a syngas yield of 8.5 mmol/g, and CO yield of 4.2 mmol/g in CO₂ decomposition. A-site defect engineering of the perovskite creates abundant oxygen vacancies and enhances oxygen storage capacity (OSC). Co-doping of the B-site of Sr_0.98FeO_3-δ increases oxygen mobility and CH₄/CO₂ activation, resulting in high activity in the CL-DRM process. This methodology resulted in high ionic mobility and facilitated the rapid diffusion of oxygen in the bulk phase, thereby increasing the redox properties of SrFeO_3-δ. The oxygen carrier exhibits excellent structural stability and regeneration ability in successive redox cycles. This strategy offers a simple but very effective pathway to tailor OSC, oxygen mobility, and oxygen vacancies of perovskite-structured materials for chemical looping or redox-involved processes.

甲烷化学循环干重整（CL-DRM）是一种高效工艺，可将两种主要温室气体（CH4 和 CO2）转化为合成气，作为生产液体燃料的原料。目前，该技术面临的主要障碍之一是制造稳定且具有活性的氧气载体。我们通过结合 SrFeO3-δ 的 A 位缺陷和 B 位掺杂，制造出了高性能的 Sr0.98Fe0.7Co0.3O3-δ 包晶结构氧载体。在 850 °C 的等温 CL-DRM 试验中，Sr0.98Fe0.7Co0.3O3-δ 在 CH4 部分氧化反应中实现了 87% 的 CH4 转化率和 94% 的 CO 选择性，随后合成气产量为 8.5 mmol/g，CO2 分解的 CO 产量为 4.2 mmol/g。过氧化物的 A 位缺陷工程产生了大量的氧空位，提高了储氧能力（OSC）。Sr0.98FeO3-δ 的 B 位共掺杂增加了氧的迁移率和 CH4/CO2 的活化，从而在 CL-DRM 过程中产生了高活性。这种方法产生了高离子迁移率，促进了氧气在体相中的快速扩散，从而提高了 SrFeO3-δ 的氧化还原特性。氧载体在连续的氧化还原循环中表现出优异的结构稳定性和再生能力。这种策略为定制化学循环或氧化还原过程中的包晶结构材料的 OSC、氧迁移率和氧空位提供了一种简单但非常有效的途径。

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引用次数: 0

Deep eutectic solvent-induced controllable synthesis of bifunctional Ni–Fe–P catalysts for electrochemical water splitting 深共晶溶剂诱导可控合成用于电化学水分离的双功能 Ni-Fe-P 催化剂

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-04-10 DOI: 10.1016/j.gce.2024.04.002

Ruichang Xue , Rongrong Deng , Yan Li , Mengqiu Gao , Jiafu Wang , Qibo Zhang

Developing electrocatalysts with excellent activity, high stability, and low cost is vital for large-scale hydrogen production through electrochemical water splitting. Herein, a bifunctional Ni–Fe–P catalyst in situ grown on Fe foam (Ni–Fe–P/FF) is developed by a simple one-step solvothermal process in the deep eutectic solvent (DES) of ethylene glycol and choline chloride (named Ethaline). The unique solvent environment of Ethaline assisted with the regulating effect of the introduced Fe(III) ions shows an essential role in governing the preparation process. The developed Ni–Fe–P/FF acts as the efficient bifunctional electrocatalyst for water splitting in 1.0 M KOH, requiring overpotentials of 82 mV (229 mV) and 263 mV (370 mV) to deliver 10 mA cm⁻² (100 mA cm⁻²) for oxygen and hydrogen evolution reactions, respectively. Furthermore, the self-supported catalyst-assembled electrolyzer also exhibits good catalytic performance with a low voltage of 1.83 V to drive 100 mA cm⁻² and good stability over 100 h. This work offers a facile approach to fabricating high-performance bifunctional Ni–Fe–P electrocatalysts to catalyze water splitting.

开发具有优异活性、高稳定性和低成本的电催化剂对于通过电化学水分离大规模制氢至关重要。在此，我们在乙二醇和氯化胆碱的深共晶溶剂（DES）（命名为乙酞）中，通过简单的一步溶剂热法，开发出了一种在铁泡沫上原位生长的双功能镍-芴-P 催化剂（镍-芴-P/FF）。乙酞的独特溶剂环境以及引入的铁（III）离子的调节作用在制备过程中发挥了重要作用。所开发的 Ni-Fe-P/FF 可作为高效的双功能电催化剂在 1.0 M KOH 中进行水分离，氧气和氢气进化反应分别需要 82 mV (229 mV) 和 263 mV (370 mV) 的过电位才能达到 10 mA cm-2 (100 mA cm-2)。此外，自支撑催化剂组装的电解槽也表现出良好的催化性能，只需 1.83 V 的低电压即可驱动 100 mA cm-2 的反应，并且在 100 小时内具有良好的稳定性。这项工作为制造催化水分离的高性能双功能 Ni-Fe-P 电催化剂提供了一种简便的方法。

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引用次数: 0

Deep eutectic solvents for fractionation and valorization of lignocellulose 用于木质纤维素分馏和增值的深度共晶溶剂

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-04-06 DOI: 10.1016/j.gce.2024.04.001

Yansai Bao, Yang Wang, Chuanyu Yan, Zhimin Xue

Deep eutectic solvents (DESs) are recognized as an emerging green solvent that can be applied to lignocellulosic biomass fractionation and valorization. A deep understanding of the physicochemical properties of DESs is of great significance to the development of biomass processing technology. Meanwhile, the importance of DESs is manifested by an increasing number of value-added chemicals derived from lignocellulose in DESs. This review focuses on the physicochemical properties of different types of DESs as well as examples of their application to lignocellulosic fractionation. Additionally, recent advancements in research on converting products from DESs fractionation into bio-based materials are highlighted. Potential obstacles and prospects for integrating DESs into biomass processing are also discussed.

深共晶溶剂（DESs）被认为是一种新兴的绿色溶剂，可用于木质纤维素生物质的分馏和增值。深入了解 DESs 的物理化学特性对生物质加工技术的发展具有重要意义。同时，DESs 的重要性还表现在越来越多的增值化学品从 DESs 中的木质纤维素中提取出来。本综述重点介绍了不同类型 DES 的物理化学特性及其在木质纤维素分馏中的应用实例。此外，还重点介绍了将 DESs 分馏产品转化为生物基材料的最新研究进展。还讨论了将 DESs 纳入生物质加工的潜在障碍和前景。

引用次数: 0

The different structure and properties of protic ionic liquid in alcohol from acid and base: butylammonium butyrate mixing with butanol, butyric acid, and butylamine respectively 原离子液体在酒精中与酸和碱的不同结构和性质：丁酸丁铵分别与丁醇、丁酸和丁胺的混合物

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-04-04 DOI: 10.1016/j.gce.2024.03.005

Xuan Zhang , Yue Zhang , Haoran Li , Jia Yao

Solvents are commonly added into protic ionic liquids (PILs) to reduce viscosity in practical applications. Understanding the relationship between the structure and properties of PILs mixed with solvents is also essential for tailoring specific applications, however, such research is limited. In this study, we measured and compared the density, viscosity, and conductivity of three mixed systems: n-butylammonium butyrate ionic liquid (PIL) mixing with N-butyric acid (PrCOOH), PIL-N-butylamine (BuNH₂), and PIL-N-butanol (BuOH). Small- and wide-angle X-ray scattering (S/WAXS), molecular dynamics (MD) simulation, and electron paramagnetic resonance (EPR) techniques were used to explore their inherent structural differences. The results indicate that the properties of the PIL-BuOH and PIL-PrCOOH systems exhibit more overall similarity in trends compared to the PIL-BuNH₂ system. However, when the molar fraction of alcohol or acid exceeds 0.8, structural differences between the two systems lead to the differences in properties. The hydrogen bond network between the BuOH molecules outside the ion cluster leads to higher viscosity and conductivity than the PIL-PrCOOH system. However, the strong hydrogen bond between PrCOOH and anions will replace the position of cations and form spherical clusters. This research highlights how distinct structures influence diverse properties, providing deeper insights into the structure-property relationship.

在实际应用中，为了降低粘度，通常会在原生离子液体（PIL）中添加溶剂。了解与溶剂混合的 PIL 的结构和性质之间的关系对于定制特定应用也是至关重要的，但这方面的研究还很有限。在本研究中，我们测量并比较了三种混合体系的密度、粘度和电导率：与 N-丁酸（PrCOOH）混合的丁酸正丁基铵离子液体（PIL）、PIL-N-丁胺（BuNH2）和 PIL-N-丁醇（BuOH）。研究采用了小角和广角 X 射线散射（S/WAXS）、分子动力学（MD）模拟和电子顺磁共振（EPR）技术来探索它们内在的结构差异。结果表明，与 PIL-BuNH2 体系相比，PIL-BuOH 和 PIL-PrCOOH 体系的性质在趋势上表现出更大的整体相似性。然而，当醇或酸的摩尔分数超过 0.8 时，两种体系之间的结构差异就会导致性质的不同。离子簇外的 BuOH 分子之间的氢键网络导致粘度和电导率高于 PIL-PrCOOH 体系。然而，PrCOOH 与阴离子之间的强氢键会取代阳离子的位置，形成球形离子簇。这项研究强调了不同的结构如何影响不同的性质，为深入了解结构与性质之间的关系提供了依据。

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引用次数: 0

Numerical study on performance optimization and flow mechanism of a new cyclone separator 新型旋风分离器性能优化和流动机理的数值研究

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-29 DOI: 10.1016/j.gce.2024.03.006

Mengjing Feng , Chengmin Gui , Yangfan Zhou , Zhigang Lei

This study proposed a new cyclone separator, using a designed nozzle inside the traditional cyclone separator, which significantly improved the efficiency of separating fine particles while maintaining an essentially unchanged pressure drop. Firstly, computational fluid dynamics (CFD) was used to compare the flow characteristics of the new cyclone separator with those of the traditional cyclone separator. On this basis, this study comprehensively investigated the pressure drop and separation efficiency of two separators under varying working conditions. The new separator achieved a separation efficiency for particles with a particle size of 1 μm that was approximately 45% higher than that of the traditional separator when the inlet velocity was 2–10 m/s. Besides, the pressure drop of the cyclone separator remained unchanged while the separation efficiency increased by 46% at an inlet flow rate of 2 m/s. The influence of the outlet area of the nozzle inside the new cyclone separator on the separation efficiency and pressure drop was analyzed, and the outlet area of the nozzle with the best overall performance was determined. It was found that the overall performance of the new cyclone separator is optimal when the nozzle outlet area is S/f = 2 cm. Finally, an energy-saving cyclone separator with high separation efficiency was developed through an in-depth study of the variation of particle motion configuration with time. It is worth noting that this study provides a guidance for the flow field analysis and geometry optimization of new gas-solid separators, not limited to cyclone separators.

本研究提出了一种新型旋风分离器，它在传统旋风分离器内部设计了一个喷嘴，在保持压降基本不变的情况下，显著提高了分离细颗粒的效率。首先，利用计算流体动力学（CFD）比较了新型旋风分离器与传统旋风分离器的流动特性。在此基础上，本研究全面考察了两种分离器在不同工作条件下的压降和分离效率。当入口速度为 2-10 m/s 时，新型分离器对粒径为 1 μm 的颗粒的分离效率比传统分离器高出约 45%。此外，当入口流速为 2 m/s 时，旋风分离器的压降保持不变，而分离效率却提高了 46%。分析了新型旋风分离器内部喷嘴出口面积对分离效率和压降的影响，并确定了综合性能最佳的喷嘴出口面积。结果发现，当喷嘴出口面积为 S/f = 2 cm 时，新型旋风分离器的整体性能最佳。最后，通过深入研究颗粒运动构型随时间的变化，开发出一种具有高分离效率的节能旋风分离器。值得注意的是，本研究为新型气固分离器的流场分析和几何优化提供了指导，而不仅限于旋风分离器。

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引用次数: 0

Near-infrared long-lifetime emission via triplet-to-singlet Förster resonance energy transfer 通过三重子到星子的佛斯特共振能量转移实现近红外长寿命发射

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-22 DOI: 10.1016/j.gce.2024.03.004

Ruihong Liu , Dongzhi Liu , Xiang Ma

Here, an innovative approach to achieve near-infrared (NIR) long-lived circularly polarized luminescence (CPL) in amorphous organic polymer materials was achieved. By co-doping bi-naphthalene derivative R/S-BPN as energy donors with porphyrin derivative TPPOH as energy acceptor into PVA polymer matrix, the NIR long-lifetime fluorescence was successfully realized through the principles of triplet-to-singlet Förster resonance energy transfer (TS-FRET). Photophysical characterizations revealed distinct room temperature phosphorescence (RTP) emission peaks and phosphorescence lifetimes for different donor-acceptor ratios. The TS-FRET process facilitated extended lifetime and red-shifted emission of the acceptor TPPOH. Moreover, employing the chiral donor R/S-BPN as chiral seeds to establish chiral environments facilitated the achievement of near-infrared CPL. These findings offer a novel and practical strategy for achieving long-wavelength and long-lifetime CPL fluorescence without complex molecular engineering, presenting potential applications in various technological fields.

本文采用创新方法在非晶有机聚合物材料中实现了近红外（NIR）长寿命圆偏振发光（CPL）。通过将双萘衍生物 R/S-BPN 作为能量供体与卟啉衍生物 TPPOH 作为能量受体共同掺杂到 PVA 聚合物基体中，利用三重子-子午佛斯特共振能量转移（TS-FRET）原理，成功实现了近红外长寿命荧光。光物理特性分析表明，在不同的供体-受体比例下，室温磷光（RTP）发射峰和磷光寿命各不相同。TS-FRET 过程有助于延长受体 TPPOH 的寿命和红移发射。此外，采用手性供体 R/S-BPN 作为手性种子来建立手性环境，有助于实现近红外 CPL。这些发现提供了一种新颖实用的策略，无需复杂的分子工程就能实现长波长和长寿命的 CPL 荧光，有望应用于各种技术领域。

引用次数: 0

Outside Back Cover 封底外侧

Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-15 DOI: 10.1016/S2666-9528(24)00014-1

引用次数: 0

OFC: Outside Front Cover OFC：封面外侧

Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-15 DOI: 10.1016/S2666-9528(24)00006-2

引用次数: 0

Boosting visible-light-driven hydrogen evolution through Pt site anchored 2D/2D heterostructure catalyst: Cd-TCPP(Pt)@CdS 通过锚定 Pt 位点的 2D/2D 异质结构催化剂促进可见光驱动的氢气进化：Cd-TCPP(Pt)@CdS

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-15 DOI: 10.1016/j.gce.2024.03.002

Guo-Wei Guan, Yi-Tao Li, Li-Ping Zhang, Su-Tao Zheng, Si-Chao Liu, Hao-Ling Lan, Qing-Yuan Yang

Solar-powered water splitting is an up-and-coming method for hydrogen production. Still, it faces several challenges, including improving light responsiveness, maximizing utilization of photocatalyst active sites, and effectively utilizing photo-induced carriers to prevent low hydrogen production. In this research, we propose an approach for designing a 2D/2D heterostructure catalyst, the Cd-TCPP(Pt)@CdS, which consists of 2D CdS nanosheets (NSs) and a 2D metal-organic framework (MOF) with Pt active sites (Cd-TCPP(Pt)), aiming to achieve highly efficient visible-light-driven hydrogen evolution. Firstly, CdS NSs exhibit excellent responsiveness to visible light, ensuring robust generation of photo-induced carriers. Secondly, the 2D MOF provides abundant Pt active sites, enhancing electron utilization and reducing the energy barrier for proton reduction. Compared to pure CdS NSs (which demonstrate a hydrogen production activity of 1220 μmol/g/h), the newly designed 2D/2D composite catalyst Cd-TCPP(Pt)@CdS exhibits an activity of 13,434 μmol/g/h, representing an 11-fold increase. Impressively, Cd-TCPP(Pt)@CdS maintains a high activity of 3062 μmol/g/h even under sunlight. Density functional theory (DFT) calculations were employed to investigate the principle of proton reduction. The suitable bandgap of CdS and energy gap of 2D Cd-TCPP(Pt) contribute to their strong interaction and consequently higher efficiency in hydrogen evolution. The Pt-single atom (Pt-SA) also provides sites with low free energy for proton reduction, contributing to improved activity. The photocatalytic performance of Cd-TCPP(Pt)@CdS NSs composites demonstrates a synergistic effect between the 2D inorganic semiconductor and the 2D MOF containing the Pt-site, resulting in enhanced utilization of photo-induced carriers and atoms.

太阳能水分离是一种新兴的制氢方法。然而，它仍然面临着一些挑战，包括提高光响应速度、最大限度地利用光催化剂活性位点以及有效利用光诱导载流子以防止氢气产量过低。在本研究中，我们提出了一种设计二维/二维异质结构催化剂 Cd-TCPP(Pt)@CdS 的方法，该催化剂由二维 CdS 纳米片（NSs）和具有铂活性位点的二维金属有机框架（MOF）（Cd-TCPP(Pt)）组成，旨在实现可见光驱动的高效氢气进化。首先，CdS NSs 对可见光具有极佳的响应性，确保了光诱导载流子的稳健生成。其次，二维 MOF 提供了丰富的铂活性位点，提高了电子利用率，降低了质子还原的能量障碍。与纯 CdS NSs（其制氢活性为 1220 μmol/g/h）相比，新设计的二维/二维复合催化剂 Cd-TCPP(Pt)@CdS 的活性为 13,434 μmol/g/h，提高了 11 倍。令人印象深刻的是，即使在阳光下，Cd-TCPP(Pt)@CdS 也能保持 3062 μmol/g/h 的高活性。密度泛函理论（DFT）计算用于研究质子还原原理。CdS 的合适带隙和二维 Cd-TCPP（Pt）的能隙有助于它们的强相互作用，从而提高氢气进化的效率。铂单原子（Pt-SA）也为质子还原提供了自由能较低的位点，从而提高了活性。Cd-TCPP(Pt)@CdS NSs 复合材料的光催化性能表明，二维无机半导体与含有铂位点的二维 MOF 之间存在协同效应，从而提高了光诱导载流子和原子的利用率。

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引用次数: 0

Flexible photosensors based on photothermal conversion 基于光热转换的柔性光传感器

IF 9.1 Q1 ENGINEERING, CHEMICAL

Green Chemical Engineering

Pub Date : 2024-03-15 DOI: 10.1016/j.gce.2024.03.001

Beihang Xu, Yao An, Jinghao Zhu, Yonglin He

The perception of light is crucial for humans to explore the external world. However, challenges of current planar photosensors include inherent limitations in depth of field and field of view. Flexible electronic devices offer a solution to this issue by allowing adaptation to curved surfaces, ensuring stable interfaces and excellent signal quality. Compared to photoelectric sensors, flexible photosensors based on photothermal conversion can respond to a wider spectrum of light, simplify design processes, and overcome issues such as instability and high toxicity. The review introduces progress on the flexible photosensors based on photothermal conversion, and summarizes the combination of photothermal conversion with pyroelectric, thermoelectric, and thermoresistive effects, allowing for the conversion of light signals into thermal signals and then into electric signals. Additionally, the review outlines the challenges for future research in this field.

对光的感知对于人类探索外部世界至关重要。然而，目前的平面光传感器面临的挑战包括景深和视场的固有限制。柔性电子器件可以适应曲面，确保稳定的接口和出色的信号质量，从而为这一问题提供了解决方案。与光电传感器相比，基于光热转换的柔性光传感器可以响应更宽的光谱，简化设计流程，并克服不稳定性和高毒性等问题。综述介绍了基于光热转换的柔性光传感器的研究进展，总结了光热转换与热释电效应、热电效应和热阻效应的结合，从而实现了光信号到热信号再到电信号的转换。此外，综述还概述了该领域未来研究面临的挑战。

引用次数: 0

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