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Enhancing carbon dioxide reduction electrocatalysis by tuning metal-support interactions: a first principles study 通过调节金属-载体相互作用增强二氧化碳还原电催化:第一性原理研究
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-09-01 DOI: 10.1016/j.gce.2022.08.003
Riming Hu , Yanan Yu , Yongcheng Li , Yiran Wang , Jiaxiang Shang , Xuchuan Jiang

The electrochemical reduction of CO2 is an extremely potential technique to achieve the goal of carbon neutrality, but the development of electrocatalysts with high activity, excellent product selectivity, and long-term durability remains a great challenge. Herein, the role of metal-supports interaction (MSI) between different active sites (including single and bimetallic atom sites consisting of Cu and Ni atoms) and carbon-based supports (including C2N, C3N4, N-coordination graphene, and graphdiyne) on catalytic activity, product selectivity, and thermodynamic stability towards CO2 reduction reaction (CRR) is systematically investigated by first principles calculations. Our results show that MSI is mainly related to the charge transfer behavior from metal sites to supports, and different MSI leads to diverse magnetic moments and d-band centers. Subsequently, the adsorption and catalytic performance can be efficiently improved by tuning MSI. Notably, the bimetallic atom supported graphdiyne not only exhibits a better catalytic activity, higher product selectivity, and higher thermodynamic stability, but also effectively inhibits the hydrogen evolution reaction. This finding provides a new research idea and optimization strategy for the rational design of high-efficiency CRR catalysts.

电化学还原CO2是实现碳中和目标的一项极具潜力的技术,但开发具有高活性、优异的产品选择性和长期耐久性的电催化剂仍然是一个巨大的挑战。在此,不同活性位点(包括由Cu和Ni原子组成的单原子和双金属原子位点)与碳基载体(包括C2N、C3N4、N-配位石墨烯和石墨烯)之间的金属-载体相互作用(MSI)对催化活性、产物选择性,并通过第一性原理计算系统地研究了对CO2还原反应(CRR)的热力学稳定性。我们的结果表明,MSI主要与从金属位点到载体的电荷转移行为有关,不同的MSI导致不同的磁矩和d带中心。随后,可以通过调节MSI来有效地提高吸附和催化性能。值得注意的是,双金属原子负载的石墨炔不仅表现出更好的催化活性、更高的产物选择性和更高的热力学稳定性,而且有效地抑制了析氢反应。这一发现为高效CRR催化剂的合理设计提供了新的研究思路和优化策略。
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引用次数: 0
Highly efficient separation of benzene + cyclohexane mixtures by extraction combined extractive distillation using imidazolium-based dicationic ionic liquids 咪唑基双离子液体萃取-萃取-精馏高效分离苯+环己烷混合物
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-09-01 DOI: 10.1016/j.gce.2022.07.003
Wanxiang Zhang , Wuji Zhao , Shuhang Ren , Yucui Hou , Weize Wu

Benzene (BEN) and cyclohexane (CYH), which have very close boiling points and a binary azeotrope, are the most difficult binary components in the separation of aromatic and non-aromatic hydrocarbons. This study further explored the separation mechanism and industrial application prospects of BEN ​+ ​CYH mixtures separated by a dicationic ionic liquid (DIL) [C5(MIM)2][NTf2]2 based on experimental research. The calculation results of the Conductor-like Screening model Segment Activity Coefficient (COSMO-SAC) model show that selectivity and solvent capacity of the DIL are significantly improved. The effects of different anions and cations on the microstructure distribution and diffusion behavior of BEN ​+ ​CYH system were investigated by quantum chemistry (QC) calculations and molecular dynamics (MD) simulations. The results indicate that the anion [NTf2] has low polarity, uniform charge distribution, and a dual role of hydrogen bonding and π-π bonding, and the cation [C5(MIM)2]2+ has stronger interaction with BEN and higher selectivity than conventional cations. The liquid-liquid extraction and extractive distillation (LLE-ED) process using an optimized 65 mol/mol DIL ​+ ​35 mol/mol H2O mixed solution as the extractant was proposed, which solved the problem of low product purity in the LLE process and high energy consumption in the ED process. Under the best operating conditions, the purity of CYH product was 99.9%, the purity of BEN product was 99.6%, the recovery rate of BEN reached 99.9%, and the recovery rate of DIL reached 99.9%. The heat-integrated LLE-ED process reduced total annual cost by 21.6%, and reduced CO2 emissions by 48.0%, which has broad industrial application prospects.

苯(BEN)和环己烷(CYH)具有非常接近的沸点和二元共沸物,是芳烃和非芳烃分离中最困难的二元组分。本研究进一步探讨了苯的分离机理及工业应用前景​+​基于实验研究,通过二元离子液体(DIL)[C5(MIM)2][NTf2]2分离的CYH混合物。类导体筛选模型分段活性系数(COSMO-SAC)模型的计算结果表明,DIL的选择性和溶剂容量显著提高。不同阴离子和阳离子对苯甲酸微观结构分布和扩散行为的影响​+​通过量子化学(QC)计算和分子动力学(MD)模拟研究了CYH体系。结果表明,阴离子[NTf2]−极性低,电荷分布均匀,具有氢键和π-π键的双重作用,阳离子[C5(MIM)2]2+与苯的相互作用更强,选择性高于传统阳离子。使用优化的65mol/mol DIL的液-液萃取和萃取蒸馏(LLE-ED)工艺​+​提出了35mol/mol H2O混合溶液作为萃取剂,解决了LLE工艺中产品纯度低、ED工艺能耗高的问题。在最佳操作条件下,CYH产品纯度为99.9%,BEN产品纯度为99.6%,BEN回收率达到99.9%,DIL回收率达到99.9%.热集成LLE-ED工艺使年总成本降低21.6%,CO2排放量降低48.0%,具有广阔的工业应用前景。
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引用次数: 8
Hydrothermal carbonization pretreatment makes a remarkable difference in activation of rice and lettuce in food waste 水热碳化预处理对餐厨垃圾中的大米和生菜的活化效果有显著影响
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-25 DOI: 10.1016/j.gce.2023.08.004

Cooked rice and the vegetables like lettuce are common kitchen waste, which are carbonaceous materials and have the potential as feedstock for the production of activated carbon. Cooking is similar to hydrothermal treatment (HTC), which might impact the subsequent activation of kitchen waste. In this study, the HTC of lettuce, rice, or their mixture and the activation of the resulting hydrochars were conducted. The results indicated that cross-polymerization between the N-containing organics from lettuce and the sugar derivatives from rice took place in their co-HTC, which significantly increased the hydrochar yield. Activation of the hydrochar from the co-HTC generated the AC with a yield of 2 times that from direct activation of mixed lettuce/rice. However, the co-HTC facilitated aromatization, reducing reactivity with K2C2O4 in activation and producing the AC with main micropores and low specific surface area. Activation of the hydrochar from HTC of rice followed the above trend, while that from lettuce was the opposite. The organics in lettuce were thermally unstable and could not undergo sufficient aromatization. The activation of hydrochar from HTC of lettuce thus generated the AC with the lowest yield, but the highest specific surface area (1684.9 m2/g), abundant mesopores, and superior capability for adsorption of tetracycline. However, the environmental impacts and energy consumption for the production of AC from the hydrochar of lettuce were higher than that from hydrochar of co-HTC.

煮熟的米饭和莴苣等蔬菜是常见的厨房垃圾,它们是碳质材料,有可能成为生产活性炭的原料。烹饪类似于水热处理(HTC),可能会影响厨余垃圾的后续活化。本研究对莴苣、大米或它们的混合物进行了水热处理,并对产生的水成碳进行了活化。结果表明,莴苣中的含氮有机物和大米中的糖衍生物在它们的共热处理过程中发生了交叉聚合,从而显著提高了水炭产率。活化来自共 HTC 的水炭产生的 AC 产量是直接活化莴苣/大米混合水炭产量的 2 倍。不过,共四氯化碳促进了芳香化,降低了活化过程中与 K2C2O4 的反应性,生成的 AC 主要有微孔,比表面积较低。水稻 HTC 水炭的活化遵循上述趋势,而莴苣则相反。莴苣中的有机物热不稳定,无法充分芳香化。因此,活化莴苣 HTC 中的水炭生成的 AC 产率最低,但比表面积(1684.9 m2/g)最高,中孔丰富,对四环素的吸附能力更强。不过,用莴苣水煤灰生产 AC 对环境的影响和能耗都高于用共四氯化碳水煤灰生产 AC。
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引用次数: 0
A review on the chemo-catalytic conversion of cellulose to bio-ethanol 纤维素化学催化转化为生物乙醇研究进展
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-22 DOI: 10.1016/j.gce.2023.08.002

While the industry has produced sugar-derived ethanol from the conventional method of fermentation for hundreds of years, other effective routes involving the direct transformation of carbohydrates still remain extremely rare. Very recently, an innovative chemo-catalytic method driven by the aqueous-phase catalysis was created for the synthesis of cellulosic ethanol, making a great breakthrough in the common ways as it can theoretically utilize all of the carbon atoms in sugars with faster kinetics; up to now, results from the relevant studies have been accumulated to a certain extent, but the periodic conclusions in this field are unfortunately absent. For this reason, this work tries to offer an overview of the cellulosic ethanol produced by chemo-catalytic routes, highlighting the present knowledge in relation to the technical efficiency, catalytic mechanisms as well as practical applications. At first, the advanced progress on the increasing efficiency from a varied type of catalytic systems are extensively discussed, which involves the specific functions of hybrid components from different strategies; meanwhile, the general influences of processing conditions, such as the hydrothermal severity and aqueous environments, are also identified. Subsequently, possible mechanisms behind the chemo-catalytic processes are widely elaborated by analyzing a number of experimental cases associated with the reaction network and its kinetic models. After that, the actual effects of this technique on the real biomass are collected to identify the positive/negative interactions between multiple components, together with the potential solutions on the semi-continuous processes of pilot scale application. The techno-economic analysis (TEA) is also calculated and compared with other similar methods, such as fermentation and gasification. Finally, several proposals aimed at upgrading the whole chain of chemo-catalytic processes are clearly provided, which may function as a guideline for future studies on the production of bio-ethanol from lignocellulosic materials.

数百年来,业界一直采用传统的发酵法生产糖乙醇,但其他直接转化碳水化合物的有效途径仍然极为罕见。最近,一种由水相催化驱动的创新型化学催化方法被用于合成纤维素乙醇,这种方法在理论上可以以更快的动力学利用糖类中的所有碳原子,从而在普通方法上取得了重大突破;迄今为止,相关研究的成果已积累到一定程度,但遗憾的是,该领域还缺乏阶段性结论。因此,本研究试图概述通过化学催化路线生产纤维素乙醇的情况,重点介绍与技术效率、催化机制和实际应用有关的现有知识。首先,文章广泛讨论了各种类型催化系统在提高效率方面取得的先进进展,其中涉及不同策略中混合成分的特定功能;同时,文章还指出了水热严重程度和水环境等加工条件的一般影响。随后,通过分析与反应网络及其动力学模型相关的大量实验案例,广泛阐述了化学催化过程背后的可能机制。之后,收集了该技术对实际生物质的实际影响,以确定多种成分之间的正/负相互作用,以及在中试规模应用的半连续过程中的潜在解决方案。还计算了技术经济分析(TEA),并与发酵和气化等其他类似方法进行了比较。最后,还明确提出了几项旨在提升整个化学催化工艺链的建议,这些建议可作为今后利用木质纤维素材料生产生物乙醇的研究指南。
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引用次数: 0
Enhanced termination of zinc and cadmium ions from wastewater employing plain and chitosan-modified mxenes: synthesis, characterization, and adsorption performance 壳聚糖和壳聚糖改性mxenes对废水中锌和镉离子的增强封端:合成、表征和吸附性能
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-22 DOI: 10.1016/j.gce.2023.08.003

Zinc and cadmium pollutants cause a significant environmental effect that cannot be ignored. Due to their considerable amount in an aqueous environment, industries are seeking suitable adsorbents that are environmentally friendly and inexpensive for removing metals from wastewater before disposing of them in surface waters. This research employed original MXene (MX) and chitosan-modified MXene (CSMX) to extract zinc (Zn(II)) and cadmium (Cd(II)) metal ions from water-based solutions. The composite material produced was analyzed using techniques such as X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), Fourier Transform Infrared Spectroscopy (FTIR), and Brunauer-Emmett-Teller (BET). The effects of contact duration, pH of the solution, and initial concentration of metal ions on the adsorption process of Zn(II) and Cd(II) onto both MX and CSMX composites were investigated. MX and prepared CSMX composite presented a high adsorption capacity for both studied heavy metals, which were 91.55 and 73.82 mg/g for Zn(II) and Cd(II) onto MX, 106.84 and 93.07 mg/g for Cd(II) and Zn(II) onto CSMX composite, respectively. Furthermore, the maximum competitive adsorption capacities for Zn(II) onto MX and CSMX composites are 77.29 and 93.47 mg/g, and for are Cd(II) 60.30 and 79.66 mg/g, respectively. Hence, the removal capacities for both single and competitive metal ions were superior to CSMX composite. However, the adsorption capacities after five successive regeneration sequences were only dropped by 13.2% for Zn(II) and 17.4% for Cd(II) onto the CSMX composite compared to the first cycle. These results confirm that both metals could be efficiently terminated from wastewater, which makes the prepared CSMX composite a favorable candidate adsorbent in practical applications.

锌和镉污染物对环境的影响不容忽视。由于锌和镉在水环境中的含量相当大,各行各业都在寻找既环保又廉价的合适吸附剂,以便在将金属排入地表水之前将其从废水中去除。本研究采用原始 MXene(MX)和壳聚糖改性 MXene(CSMX)从水基溶液中提取锌(Zn(II))和镉(Cd(II))金属离子。利用 X 射线衍射 (XRD)、扫描电子显微镜 (SEM)、傅立叶变换红外光谱 (FTIR) 和布鲁瑙尔-艾美特-泰勒 (BET) 等技术对制备的复合材料进行了分析。研究了接触时间、溶液 pH 值和金属离子初始浓度对 MX 和 CSMX 复合材料吸附 Zn(II) 和 Cd(II) 过程的影响。MX 和制备的 CSMX 复合材料对所研究的两种重金属都有很高的吸附容量,MX 对 Zn(II) 和 Cd(II) 的吸附容量分别为 91.55 和 73.82 mg/g,CSMX 复合材料对 Cd(II) 和 Zn(II) 的吸附容量分别为 106.84 和 93.07 mg/g。此外,MX 和 CSMX 复合材料对 Zn(II) 的最大竞争吸附容量分别为 77.29 和 93.47 毫克/克,对 Cd(II) 的最大竞争吸附容量分别为 60.30 和 79.66 毫克/克。因此,CSMX 复合材料对单一金属离子和竞争性金属离子的去除能力都更胜一筹。然而,与第一个循环相比,CSMX 复合材料在连续五个再生循环后对 Zn(II) 和 Cd(II) 的吸附能力分别只下降了 13.2% 和 17.4%。这些结果证实,废水中的这两种金属都能被有效地去除,这使得制备的 CSMX 复合材料在实际应用中成为一种有利的候选吸附剂。
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引用次数: 0
Ionic liquid driven nanostructure self-assembly in organic mixed ionic-electronic conductors 离子液体驱动的有机混合离子-电子导体纳米结构自组装
IF 9.1 Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-05 DOI: 10.1016/j.gce.2023.08.001
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引用次数: 0
The stability of MOFs in aqueous solutions—research progress and prospects mof在水溶液中的稳定性——研究进展与展望
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-08-01 DOI: 10.1016/j.gce.2023.07.004
Yang An , Xinling Lv , Weiyi Jiang , Lingling Wang , Yuxin Shi , Xinxin Hang , Huan Pang

Metal-organic frameworks (MOFs) are favored in the fields of adsorption, separation, catalysis, electrochemistry, and magnetism due to their advantages of large specific surface area, high porosity, controllable pore size adjustment, and dispersion of metal active sites. The application of MOFs involves multiple fields, which requires that MOFs have good water stability, as gaseous and liquid water inevitably exist in industrial processes. In this paper, the research status of the stability of MOFs in aqueous solutions was reviewed in recent years, including the design and synthesis, the influencing factors, and the applications of MOFs in water stability.

金属有机框架(MOFs)因其比表面积大、孔隙率高、孔径调节可控、金属活性位点分散等优点,在吸附、分离、催化、电化学、磁学等领域备受青睐。MOFs 的应用涉及多个领域,由于工业生产过程中不可避免地存在气态和液态水,这就要求 MOFs 具有良好的水稳定性。本文综述了近年来MOFs在水溶液中稳定性的研究现状,包括MOFs的设计与合成、影响因素以及在水稳定性方面的应用。
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引用次数: 0
Application of efficient and sustainable freeze-dissolving technology in manufacturing of KHCO3 ultrafine particles 高效可持续冷冻溶解技术在KHCO3超细颗粒制备中的应用
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-28 DOI: 10.1016/j.gce.2023.07.003
Jiaqi Luo , Qifan Su , Qiushuo Yu , Xinyue Zhai , Yuan Zou , Huaiyu Yang

The development of ultrafine particles provided a new way to solve problems in the fields of energy, environment, and medicine, and had become one of the most promising technologies. Therefore, the application of ultrafine particles required the development of cleaner, greener, and more efficient preparation methods. The new freeze-dissolving technology has been applied in manufacturing of KHCO3 ultrafine particles, with an aqueous solution of 0.02–0.1 g KHCO3/g water. Frozen ice particles were formed after dripping the solution into liquid nitrogen. The antisolvent ethanol was used to dissolve the ice spherical template at a temperature below 273.15 K, and the pre-formed KHCO3 ultrafine particles inside the ice template remained in the ethanol aqueous solution. The ice particles were put into the freeze dryer to isolate the ultrafine KHCO3 particles. Compared with the particles produced with traditional freeze-drying technology, the ultrafine powder/particles produced by the freeze-dissolving technology were smaller with narrower size distribution. The freeze-dissolving technology has demonstrated a much more sustainable and efficient manufacturing process than the traditional freeze-drying process. In addition, the influence of the concentrations of KHCO3 and the sizes of ice particles were investigated with the discussions of mechanisms.

超微粒子的开发为解决能源、环境和医学领域的问题提供了新的途径,已成为最有前途的技术之一。因此,超微粒子的应用需要开发更清洁、更环保、更高效的制备方法。新的冷冻溶解技术已应用于 KHCO3 超微粒子的制造,水溶液为 0.02-0.1 g KHCO3/g 水。将溶液滴入液氮中后形成冷冻冰粒。在低于 273.15 K 的温度下,用抗溶剂乙醇溶解冰球模板,冰模板内预先形成的 KHCO3 超细粒子留在乙醇水溶液中。将冰颗粒放入冷冻干燥机中,分离出超细 KHCO3 颗粒。与传统冷冻干燥技术生产的颗粒相比,冷冻溶解技术生产的超细粉末/颗粒更小,粒度分布更窄。与传统的冷冻干燥工艺相比,冷冻溶解技术展示了一种更可持续、更高效的生产工艺。此外,还研究了 KHCO3 浓度和冰粒大小的影响,并讨论了相关机理。
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引用次数: 0
Dendritic mesoporous silica nanoparticles for enzyme immobilization 用于酶固定化的树枝状介孔二氧化硅纳米粒子
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-20 DOI: 10.1016/j.gce.2023.07.002
Shuling Zhang , Jing Bai , Weixi Kong , Haolei Song , Yunting Liu , Guanhua Liu , Li Ma , Liya Zhou , Yanjun Jiang

Dendritic mesoporous silica nanoparticles (DMSNs) are a new class of solid porous materials used for enzyme immobilization support due to their intrinsic characteristics, including their unique open central–radial structures with large pore channels and their excellent biocompatibility. In this review, we review the recent progress in research on enzyme immobilization using DMSNs with different structures, namely, flower-like DMSNs and tree-branch-like DMSNs. Three DMSN synthesis methods are briefly compared, and the distinct characteristics of the two DMSN types and their effects on the catalytic performance of immobilized enzymes are comprehensively discussed. Possible directions for future research on enzyme immobilization using DMSNs are also proposed.

树枝状介孔二氧化硅纳米颗粒(DMSNs)是一类新型的固体多孔材料,可用于酶固定化支撑,其固有特性包括独特的开放式中心-径向结构、大孔道以及良好的生物相容性。在这篇综述中,我们回顾了利用不同结构的 DMSNs(即花朵状 DMSNs 和树枝状 DMSNs)固定酶的最新研究进展。简要比较了三种 DMSN 的合成方法,全面讨论了两种 DMSN 的不同特点及其对固定化酶催化性能的影响。此外,还提出了未来利用 DMSN 固定酶的可能研究方向。
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引用次数: 0
Can the Bass innovation diffusion model describe adsorption breakthrough curves of pharmaceutical contaminants? Bass创新扩散模型能否描述药物污染物的吸附突破曲线?
Q1 ENGINEERING, CHEMICAL Pub Date : 2023-07-18 DOI: 10.1016/j.gce.2023.07.001
Khim Hoong Chu, Mohd Ali Hashim
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引用次数: 0
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Green Chemical Engineering
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