Pub Date : 2024-02-01DOI: 10.1016/j.gee.2024.01.008
Lina Li, Yi Zhang, Gaopeng Liu, Tiange Wei, Junze Zhao, Bin Wang, Mengxia Ji, Yuanbin She, Jiexiang Xia, Huaming Li
CO2 photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect. Herein, the 5, 10, 15, 20-tetra (4-carboxyphenyl) porphyrin cobalt(II) (CoTCPP) has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite. The as-prepared CoTCPP/BiOBr-2 shows optimized photocatalytic performance for CO2 conversion into CO and CH4 upon irradiation with 300 W Xe lamp, which is 2.03 and 2.58 times compared to that of BiOBr, respectively. The introduced CoTCPP significantly enhanced light absorption properties, promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO2 molecules. The metal Co2+ at the center of the porphyrin molecules also acts as adsorption center for CO2 molecules, boosting the CO2 convert into CO and CH4. The possible mechanism of CO2 photoreduction was explored by in-situ FT-IR spectra. This work offers a new possibility for the preparation of advance photocatalysts.
将二氧化碳光降解为碳基化学品被认为是缓解能源问题和温室效应的适当途径。本文将 5、10、15、20-四(4-羧基苯基)卟啉钴(II)(CoTCPP)与 BiOBr 微球结合,形成 CoTCPP/BiOBr 复合材料。制备的 CoTCPP/BiOBr-2 在 300 W Xe 灯照射下,将 CO2 转化为 CO 和 CH4 的光催化性能达到最佳,分别是 BiOBr 的 2.03 倍和 2.58 倍。引入的 CoTCPP 显著增强了光吸收性能,促进了光生载流子的快速分离,并提高了 CO2 分子的化学吸附能力。卟啉分子中心的金属 Co2+ 也成为 CO2 分子的吸附中心,促进 CO2 转化为 CO 和 CH4。通过原位傅立叶变换红外光谱,探索了二氧化碳光生化的可能机制。这项工作为制备先进的光催化剂提供了新的可能性。
{"title":"CoTCPP integrates with BiOBr microspheres for improved solar-driven CO2 reduction performance","authors":"Lina Li, Yi Zhang, Gaopeng Liu, Tiange Wei, Junze Zhao, Bin Wang, Mengxia Ji, Yuanbin She, Jiexiang Xia, Huaming Li","doi":"10.1016/j.gee.2024.01.008","DOIUrl":"https://doi.org/10.1016/j.gee.2024.01.008","url":null,"abstract":"<p>CO<sub>2</sub> photoreduction into carbon-based chemicals has been considered as an appropriate way to alleviate the energy issue and greenhouse effect. Herein, the 5, 10, 15, 20-tetra (4-carboxyphenyl) porphyrin cobalt(II) (CoTCPP) has been integrated with BiOBr microspheres and formed the CoTCPP/BiOBr composite. The as-prepared CoTCPP/BiOBr-2 shows optimized photocatalytic performance for CO<sub>2</sub> conversion into CO and CH<sub>4</sub> upon irradiation with 300 W Xe lamp, which is 2.03 and 2.58 times compared to that of BiOBr, respectively. The introduced CoTCPP significantly enhanced light absorption properties, promoted rapid separation of photogenerated carriers and boosted the chemisorption of CO<sub>2</sub> molecules. The metal Co<sup>2+</sup> at the center of the porphyrin molecules also acts as adsorption center for CO<sub>2</sub> molecules, boosting the CO<sub>2</sub> convert into CO and CH<sub>4</sub>. The possible mechanism of CO<sub>2</sub> photoreduction was explored by <em>in-situ</em> FT-IR spectra. This work offers a new possibility for the preparation of advance photocatalysts.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"40 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139665446","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01Epub Date: 2022-11-25DOI: 10.1016/j.gee.2022.11.004
Ruijia Hu , Ming Li , Tao Shen , Xin Wang , Zhuohua Sun , Xinning Bao , Kequan Chen , Kai Guo , Lei Ji , Hanjie Ying , Pingkai Ouyang , Chenjie Zhu
Considerable progress has been made in recent years to the development of sustainable polymers from bio-based feedstocks. In this study, 100% bio-based nylons were prepared via an integrated chemical and biological process from lignocellulose. These novel nylons were obtained by the melt polymerization of 3-propyladipic acid derived from lignin and 1,5-pentenediamine/1,4-butanediamine derived from carbohydrate sugar. Central to the concept is a three-step noble metal free catalytic chemical funnelling sequence (Raney Ni mediated reductive catalytic fractionation - reductive funnelling - oxidative funnelling), which allowed for obtaining a single component 3-propyladipic acid from lignin with high efficiency. The structural and thermodynamic properties of the obtained nylons have been systematically investigated, and thus obtained transparent bio-based nylons exhibited higher Mw (>32,000) and excellent thermal stability (Td5% > 265 °C). Considering their moderate Tg and good melt strength, these transparent bio-based nylons could serve as promising functional additives or temperature-responsive materials.
{"title":"A sustainable process to 100% bio-based nylons integrated chemical and biological conversion of lignocellulose","authors":"Ruijia Hu , Ming Li , Tao Shen , Xin Wang , Zhuohua Sun , Xinning Bao , Kequan Chen , Kai Guo , Lei Ji , Hanjie Ying , Pingkai Ouyang , Chenjie Zhu","doi":"10.1016/j.gee.2022.11.004","DOIUrl":"https://doi.org/10.1016/j.gee.2022.11.004","url":null,"abstract":"<div><p>Considerable progress has been made in recent years to the development of sustainable polymers from bio-based feedstocks. In this study, 100% bio-based nylons were prepared <em>via</em> an integrated chemical and biological process from lignocellulose. These novel nylons were obtained by the melt polymerization of 3-propyladipic acid derived from lignin and 1,5-pentenediamine/1,4-butanediamine derived from carbohydrate sugar. Central to the concept is a three-step noble metal free catalytic chemical funnelling sequence (Raney Ni mediated reductive catalytic fractionation - reductive funnelling - oxidative funnelling), which allowed for obtaining a single component 3-propyladipic acid from lignin with high efficiency. The structural and thermodynamic properties of the obtained nylons have been systematically investigated, and thus obtained transparent bio-based nylons exhibited higher <em>M</em><sub>w</sub> (>32,000) and excellent thermal stability (<em>T</em><sub>d5%</sub> > 265 °C). Considering their moderate <em>T</em><sub>g</sub> and good melt strength, these transparent bio-based nylons could serve as promising functional additives or temperature-responsive materials.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"9 2","pages":"Pages 390-402"},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2468025722001753/pdfft?md5=af43c0c6f820d14ec2966209f84bc749&pid=1-s2.0-S2468025722001753-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139100434","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01Epub Date: 2023-01-02DOI: 10.1016/j.gee.2022.12.010
Yutao Liu , Liyu Chen , Lifeng Yang , Tianhao Lan , Hui Wang , Chenghong Hu , Xue Han , Qixing Liu , Jianfa Chen , Zeming Feng , Xili Cui , Qianrong Fang , Hailong Wang , Libo Li , Yingwei Li , Huabin Xing , Sihai Yang , Dan Zhao , Jinping Li
Carbon peaking and carbon neutralization trigger a technical revolution in energy & environment related fields. Development of new technologies for green energy production and storage, industrial energy saving and efficiency reinforcement, carbon capture, and pollutant gas treatment is in highly imperious demand. The emerging porous framework materials such as metal–organic frameworks (MOFs), covalent organic frameworks (COFs) and hydrogen-bonded organic frameworks (HOFs), owing to the permanent porosity, tremendous specific surface area, designable structure and customizable functionality, have shown great potential in major energy-consuming industrial processes, including sustainable energy gas catalytic conversion, energy-efficient industrial gas separation and storage. Herein, this manuscript presents a systematic review of porous framework materials for global and comprehensive energy & environment related applications, from a macroscopic and application perspective.
{"title":"Porous framework materials for energy & environment relevant applications: A systematic review","authors":"Yutao Liu , Liyu Chen , Lifeng Yang , Tianhao Lan , Hui Wang , Chenghong Hu , Xue Han , Qixing Liu , Jianfa Chen , Zeming Feng , Xili Cui , Qianrong Fang , Hailong Wang , Libo Li , Yingwei Li , Huabin Xing , Sihai Yang , Dan Zhao , Jinping Li","doi":"10.1016/j.gee.2022.12.010","DOIUrl":"10.1016/j.gee.2022.12.010","url":null,"abstract":"<div><p>Carbon peaking and carbon neutralization trigger a technical revolution in energy & environment related fields. Development of new technologies for green energy production and storage, industrial energy saving and efficiency reinforcement, carbon capture, and pollutant gas treatment is in highly imperious demand. The emerging porous framework materials such as metal–organic frameworks (MOFs), covalent organic frameworks (COFs) and hydrogen-bonded organic frameworks (HOFs), owing to the permanent porosity, tremendous specific surface area, designable structure and customizable functionality, have shown great potential in major energy-consuming industrial processes, including sustainable energy gas catalytic conversion, energy-efficient industrial gas separation and storage. Herein, this manuscript presents a systematic review of porous framework materials for global and comprehensive energy & environment related applications, from a macroscopic and application perspective.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"9 2","pages":"Pages 217-310"},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2468025722001881/pdfft?md5=24b86fcd1cea59e7401feeee6e43f18e&pid=1-s2.0-S2468025722001881-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"128774479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01Epub Date: 2022-09-22DOI: 10.1016/j.gee.2022.09.007
Fukuan Li , Weizhe Zhang , Peng Zhang , Ao Gong , Kexun Li
Electroreduction of nitrate has been gaining wide attention in recent years owing to it's beneficial for converting nitrate into benign N2 from the perspective of electrocatalytic denitrification or into value-added ammonia from the perspective of electrocatalytic NH3 synthesis. By reason of the undesired formation of ammonia is dominant during electroreduction of nitrate-containing wastewater, chloride has been widely used to improve N2 selectivity. Nevertheless, selective electroreduction of nitrate to N2 gas in chloride-containing system poses several drawbacks. In this review, we focus on the key strategies for efficiently enhancing N2 selectivity of electroreduction of nitrate in chloride-free system, including optimal selection of elements, combining an active metal catalyst with another metal, manipulating the crystalline morphology and facet orientation, constructing core–shell structure catalysts, etc. Before summarizing the strategies, four possible reaction pathways of electroreduction of nitrate to N2 are discussed. Overall, this review attempts to provide practical strategies for enhancing N2 selectivity without the aid of electrochlorination and highlight directions for future research for designing appropriate electrocatalyst for final electrocatalytic denitrification.
{"title":"Strategies of selective electroreduction of aqueous nitrate to N2 in chloride-free system: A critical review","authors":"Fukuan Li , Weizhe Zhang , Peng Zhang , Ao Gong , Kexun Li","doi":"10.1016/j.gee.2022.09.007","DOIUrl":"10.1016/j.gee.2022.09.007","url":null,"abstract":"<div><p>Electroreduction of nitrate has been gaining wide attention in recent years owing to it's beneficial for converting nitrate into benign N<sub>2</sub> from the perspective of electrocatalytic denitrification or into value-added ammonia from the perspective of electrocatalytic NH<sub>3</sub> synthesis. By reason of the undesired formation of ammonia is dominant during electroreduction of nitrate-containing wastewater, chloride has been widely used to improve N<sub>2</sub> selectivity. Nevertheless, selective electroreduction of nitrate to N<sub>2</sub> gas in chloride-containing system poses several drawbacks. In this review, we focus on the key strategies for efficiently enhancing N<sub>2</sub> selectivity of electroreduction of nitrate in chloride-free system, including optimal selection of elements, combining an active metal catalyst with another metal, manipulating the crystalline morphology and facet orientation, constructing core–shell structure catalysts, etc. Before summarizing the strategies, four possible reaction pathways of electroreduction of nitrate to N<sub>2</sub> are discussed. Overall, this review attempts to provide practical strategies for enhancing N<sub>2</sub> selectivity without the aid of electrochlorination and highlight directions for future research for designing appropriate electrocatalyst for final electrocatalytic denitrification.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"9 2","pages":"Pages 198-216"},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2468025722001388/pdfft?md5=8e7bf1c5d3c8e9fe9d0de4f6436c4233&pid=1-s2.0-S2468025722001388-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"122719775","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01Epub Date: 2022-06-11DOI: 10.1016/j.gee.2022.06.003
Rui Li , Qixuan Lin , Junli Ren , Xiaobao Yang , Yingxiong Wang , Lingzhao Kong
The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at 433 K for 1 h in the γ-butyrolactone (GBL)-H2O system, as well as the concomitant formation of 83.0% formic acid. The 13C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.
{"title":"Dealuminated Hβ zeolite for selective conversion of fructose to furfural and formic acid","authors":"Rui Li , Qixuan Lin , Junli Ren , Xiaobao Yang , Yingxiong Wang , Lingzhao Kong","doi":"10.1016/j.gee.2022.06.003","DOIUrl":"https://doi.org/10.1016/j.gee.2022.06.003","url":null,"abstract":"<div><p>The fructose-to-furfural transformation is facing major challenges in the selectivity and high efficiency. Herein, we have developed a simple and effective approach for the selective conversion of fructose to furfural using Hβ zeolite modified by organic acids for dealuminization to regulate its textural and acidic properties. It was found that citric acid-dealuminized Hβ zeolite possessed high specific surface areas, wide channels and high Brønsted acid amount, which facilitated the selective conversion of fructose to furfural with a maximum yield of 76.2% at 433 K for 1 h in the γ-butyrolactone (GBL)-H<sub>2</sub>O system, as well as the concomitant formation of 83.0% formic acid. The <sup>13</sup>C-isotope labelling experiments and the mechanism revealed that the selective cleavage of C1–C2 or C5–C6 bond on fructose was firstly occurred to form pentose or C5 intermediate by weak Brønsted acid, which was then dehydrated to furfural by strong Brønsted acid. Also this dealuminized Hβ catalyst showed the great recycling performance and was active for the conversion of glucose and mannose.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"9 2","pages":"Pages 311-320"},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2468025722000991/pdfft?md5=b1df4e09928f824fb7856274b1a2f22b&pid=1-s2.0-S2468025722000991-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139100392","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-02-01Epub Date: 2023-02-04DOI: 10.1016/j.gee.2023.01.008
Lukun Xiao , Anyi Zhao , Jie Qiu , An Liu , Sha Chen , Jinzhu Jiang , Jun Zhang , Cong Guo , Jipeng Di , Jintang Cheng , Chang Chen , Kangxin Hou , Aiping Zhang , Yan Liu , Caixia Wang
Herbal extraction residues (HERs) cause serious environmental pollution and resource waste. In this study, a novel green route was designed for the comprehensive reutilization of all components in HERs, taking Magnolia officinalis residues (MOR) as an example. The reluctant structure of MOR was first destroyed by alkali pretreatment to release the functional ingredients (magnolol and honokiol) originally remaining in MOR and to make MOR more accessible for hydrolysis. A metal–organic frame material MIL-101(Cr) with a maximum absorption capacity of 255.64 mg g−1 was synthesized to absorb the released honokiol and magnolol from the pretreated MOR solutions, and 40 g L−1 reducing sugars were obtained with 81.8% enzymatic hydrolysis rate at 10% MOR solid loading. Finally, 382 mg L−1 β-amyrin was produced from MOR hydrolysates by an engineered yeast strain. In total, 1 kg honokiol, 8 kg magnolol, and 7.64 kg β-amyrin could produce from 1 ton MOR by this cleaner process with a total economic output of 170,700 RMB.
中草药提取残渣(HERs)会造成严重的环境污染和资源浪费。本研究以厚朴提取物残渣(MOR)为例,设计了一种新型的绿色工艺路线,以实现中药提取物残渣中所有成分的综合再利用。首先通过碱预处理破坏厚朴残渣的勉强结构,释放出厚朴残渣中原本残留的功能成分(厚朴酚和厚朴酚),并使厚朴残渣更易于水解。合成了一种金属有机框架材料 MIL-101(Cr),其最大吸收能力为 255.64 mg g-1,用于吸收预处理后 MOR 溶液中释放出的红木醇和木兰醇,在 MOR 固含量为 10%的情况下,可获得 40 g L-1 的还原糖,酶水解率为 81.8%。最后,一种工程酵母菌株从 MOR 水解产物中生成了 382 mg L-1 β-amyrin。通过这种清洁工艺,从 1 吨 MOR 中总共可生产出 1 kg honokiol、8 kg magnolol 和 7.64 kg β-amyrin,总经济产出为 170,700 元人民币。
{"title":"Comprehensive reutilization of herbal waste: Coproduction of magnolol, honokiol, and β-amyrin from Magnolia officinalis residue","authors":"Lukun Xiao , Anyi Zhao , Jie Qiu , An Liu , Sha Chen , Jinzhu Jiang , Jun Zhang , Cong Guo , Jipeng Di , Jintang Cheng , Chang Chen , Kangxin Hou , Aiping Zhang , Yan Liu , Caixia Wang","doi":"10.1016/j.gee.2023.01.008","DOIUrl":"10.1016/j.gee.2023.01.008","url":null,"abstract":"<div><p>Herbal extraction residues (HERs) cause serious environmental pollution and resource waste. In this study, a novel green route was designed for the comprehensive reutilization of all components in HERs, taking <em>Magnolia officinalis</em> residues (MOR) as an example. The reluctant structure of MOR was first destroyed by alkali pretreatment to release the functional ingredients (magnolol and honokiol) originally remaining in MOR and to make MOR more accessible for hydrolysis. A metal–organic frame material MIL-101(Cr) with a maximum absorption capacity of 255.64 mg g<sup>−1</sup> was synthesized to absorb the released honokiol and magnolol from the pretreated MOR solutions, and 40 g L<sup>−1</sup> reducing sugars were obtained with 81.8% enzymatic hydrolysis rate at 10% MOR solid loading. Finally, 382 mg L<sup>−1</sup> β-amyrin was produced from MOR hydrolysates by an engineered yeast strain. In total, 1 kg honokiol, 8 kg magnolol, and 7.64 kg β-amyrin could produce from 1 ton MOR by this cleaner process with a total economic output of 170,700 RMB.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"9 2","pages":"Pages 403-412"},"PeriodicalIF":13.3,"publicationDate":"2024-02-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2468025723000249/pdfft?md5=5623ec8a351c0e866462f8b808bf15ab&pid=1-s2.0-S2468025723000249-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"132353872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-01-25DOI: 10.1016/j.gee.2024.01.006
Jiacheng Bao, Xin Sun, Ping Ning, Kai Li, Jie Yang, Fei Wang, Lei Shi, Maohong Fan
The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner. In this review, we investigate the development of industrial-waste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste. We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification, in which the active components, pore size, and phase structure can be altered. The review will discuss the potential of using industrial solid wastes, these modified materials, or synthesized materials from raw waste precursors for the removal of air pollutants, including SO2, NOx, Hg0, H2S, VOCs, and CO2. The challenges still need to be addressed to realize this potential and the prospects for future research fully. The suggests for future directions include determining the optimal composition of these materials, calculating the real reaction rate and turnover frequency, developing effective treatment methods, and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.
{"title":"Industrial solid wastes to environmental protection materials for removal of gaseous pollutants: A review","authors":"Jiacheng Bao, Xin Sun, Ping Ning, Kai Li, Jie Yang, Fei Wang, Lei Shi, Maohong Fan","doi":"10.1016/j.gee.2024.01.006","DOIUrl":"https://doi.org/10.1016/j.gee.2024.01.006","url":null,"abstract":"<p>The application of industrial solid wastes as environmentally functional materials for air pollutants control has gained much attention in recent years due to its potential to reduce air pollution in a cost-effective manner. In this review, we investigate the development of industrial-waste-based functional materials for various gas pollutant removal and consider the relevant reaction mechanism according to different types of industrial solid waste. We see a recent effort towards achieving high-performance environmental functional materials via chemical or physical modification, in which the active components, pore size, and phase structure can be altered. The review will discuss the potential of using industrial solid wastes, these modified materials, or synthesized materials from raw waste precursors for the removal of air pollutants, including SO<sub>2</sub>, NO<sub>x</sub>, Hg<sup>0</sup>, H<sub>2</sub>S, VOCs, and CO<sub>2</sub>. The challenges still need to be addressed to realize this potential and the prospects for future research fully. The suggests for future directions include determining the optimal composition of these materials, calculating the real reaction rate and turnover frequency, developing effective treatment methods, and establishing chemical component databases of raw industrial solid waste for catalysts/adsorbent preparation.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"13 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-01-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139583265","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-01-22DOI: 10.1016/j.gee.2024.01.007
Jing Fan, Zhengxing Dai, Jian Cao, Liwen Mu, Xiaoyan Ji, Xiaohua Lu
Viscosity is one of the most important fundamental properties of fluids. However, accurate acquisition of viscosity for ionic liquids (ILs) remains a critical challenge. In this study, an approach integrating prior physical knowledge into the machine learning (ML) model was proposed to predict the viscosity reliably. The method was based on 16 quantum chemical descriptors determined from the first principles calculations and used as the input of the ML models to represent the size, structure, and interactions of the ILs. Three strategies based on the residuals of the COSMO-RS model were created as the output of ML, where the strategy directly using experimental data was also studied for comparison. The performance of six ML algorithms was compared in all strategies, and the CatBoost model was identified as the optimal one. The strategies employing the relative deviations were superior to that using the absolute deviation, and the relative ratio revealed the systematic prediction error of the COSMO-RS model. The CatBoost model based on the relative ratio achieved the highest prediction accuracy on the test set (R2 = 0.9999, MAE = 0.0325), reducing the average absolute relative deviation (AARD) in modeling from 52.45% to 1.54%. Features importance analysis indicated the average energy correction, solvation-free energy, and polarity moment were the key influencing the systematic deviation.
粘度是流体最重要的基本特性之一。然而,准确获取离子液体(ILs)的粘度仍然是一项严峻的挑战。本研究提出了一种将先验物理知识整合到机器学习(ML)模型中的方法,以可靠地预测粘度。该方法基于第一原理计算确定的 16 个量子化学描述符,并将其作为 ML 模型的输入,以表示离子液体的大小、结构和相互作用。基于 COSMO-RS 模型的残差创建了三种策略作为 ML 的输出,同时还研究了直接使用实验数据的策略以进行比较。在所有策略中,比较了六种 ML 算法的性能,并确定 CatBoost 模型为最佳模型。采用相对偏差的策略优于采用绝对偏差的策略,相对比率揭示了 COSMO-RS 模型的系统预测误差。基于相对比率的 CatBoost 模型在测试集上获得了最高的预测精度(R2 = 0.9999,MAE = 0.0325),将建模中的平均绝对相对偏差(AARD)从 52.45% 降至 1.54%。特征重要性分析表明,平均能量校正、无溶解能和极性矩是影响系统偏差的关键因素。
{"title":"Hybrid Data-Driven and Physics-Based Modeling for Viscosity Prediction of Ionic Liquids","authors":"Jing Fan, Zhengxing Dai, Jian Cao, Liwen Mu, Xiaoyan Ji, Xiaohua Lu","doi":"10.1016/j.gee.2024.01.007","DOIUrl":"https://doi.org/10.1016/j.gee.2024.01.007","url":null,"abstract":"<p>Viscosity is one of the most important fundamental properties of fluids. However, accurate acquisition of viscosity for ionic liquids (ILs) remains a critical challenge. In this study, an approach integrating prior physical knowledge into the machine learning (ML) model was proposed to predict the viscosity reliably. The method was based on 16 quantum chemical descriptors determined from the first principles calculations and used as the input of the ML models to represent the size, structure, and interactions of the ILs. Three strategies based on the residuals of the COSMO-RS model were created as the output of ML, where the strategy directly using experimental data was also studied for comparison. The performance of six ML algorithms was compared in all strategies, and the CatBoost model was identified as the optimal one. The strategies employing the relative deviations were superior to that using the absolute deviation, and the relative ratio revealed the systematic prediction error of the COSMO-RS model. The CatBoost model based on the relative ratio achieved the highest prediction accuracy on the test set (R<sup>2</sup> = 0.9999, MAE = 0.0325), reducing the average absolute relative deviation (AARD) in modeling from 52.45% to 1.54%. Features importance analysis indicated the average energy correction, solvation-free energy, and polarity moment were the key influencing the systematic deviation.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"64 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-01-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139583259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Removing hydrogen sulfide (H2S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H2S into elemental sulfur. While N-doped porous carbon was applied to H2S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H2S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 gsulfur·kgcat.-1·h-1), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO2 and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.
通过选择性氧化去除硫化氢(H2S)被认为是进一步净化含硫工业的有效方法,因为它可以将残留的 H2S 完全转化为元素硫。虽然掺杂 N 的多孔碳已被应用于 H2S 选择性氧化,但合成高效稳定的掺杂 N 的碳催化剂的可持续方法仍是一个难题,限制了其未来在大规模应用中的发展。在此,我们以可重复使用的 NaCl 为模板,制备了具有大比表面积、高吡啶 N 含量和大量结构缺陷的多孔蜂窝状 N-掺杂碳催化剂,用于 H2S 选择性氧化。所制备的 NC-10-800 催化剂具有优异的催化性能(硫形成率为 784 gsulfur-kgcat.-1-h-1)、出色的稳定性(100 h)以及出色的抗水蒸气、抗 CO2 和抗氧化性能,表明其在实际工业应用中具有巨大潜力。表征结果和动力学研究表明,高温熔盐产生的大表面积和结构缺陷增强了吡啶 N 位点的暴露,从而加快了催化活性。重要的是,水溶性氯化钠模板可以很容易地从碳纳米材料中洗掉,因此下游的含盐废水随后可以重新用于碳前驱体的溶解。这种环境友好型、低成本、可重复使用的盐模板策略对掺杂 N 的碳催化剂的实际应用开发具有重要意义。
{"title":"Reusable Salt-template Strategy for Synthesis of Porous Nitrogen-rich Carbon Boosts H2S Selective Oxidation","authors":"Xu Liu, Liang Shan, Xiaoxue Sun, Tianxin Wang, Zhongqing Liu, Yuefeng Liu","doi":"10.1016/j.gee.2024.01.005","DOIUrl":"https://doi.org/10.1016/j.gee.2024.01.005","url":null,"abstract":"<p>Removing hydrogen sulfide (H<sub>2</sub>S) via the selective oxidation has been considered an effective way to further purify the indusial sulfur-containing due to it can completely transform residual H<sub>2</sub>S into elemental sulfur. While N-doped porous carbon was applied to H<sub>2</sub>S selective oxidation, a sustainable methodology for the synthesis of efficient and stable N-doped carbon catalysts remains a difficulty, limiting its future development in large-scale applications. Herein, we present porous, honeycomb-like N-doped carbon catalysts with large specific surface areas, high pyridinic N content, and numerous structural defects for H<sub>2</sub>S selective oxidation prepared using reusable NaCl as the template. The as-prepared NC-10-800 catalyst exhibits excellent catalytic performance (sulfur formation rate of 784 g<sub>sulfur</sub>·kg<sub>cat.</sub><sup>-1</sup>·h<sup>-1</sup>), outstanding stability (> 100 h), and excellent anti-water vapor, anti-CO<sub>2</sub> and anti-oxidation properties, suggesting significant potential for practical industrial application. The characterization results and kinetic study demonstrate that the large surface areas and structural defects created by the molten salt at high temperature enhance the exposure of pyridinic N sites and thus accelerate the catalytic activity. Importantly, the water-soluble NaCl template could be easily washed from the carbon nanomaterials, and thus the downstream salt-containing wastewater could be subsequently reused for the dissolution of carbon precursors. This environment-friendly, low-cost, reusable salt-template strategy has significant implications for the development of N-doped carbon catalysts for practical applications.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"107 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139471271","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-01-14DOI: 10.1016/j.gee.2024.01.004
Yanpan Li, Yanbo Zhou, Yi Zhou
Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. The ultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate both sulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidation system for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system to explore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such as ultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance were discussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.
{"title":"Ultrasonic enhancement of persulfate oxidation system governs emerging pollutants decontamination","authors":"Yanpan Li, Yanbo Zhou, Yi Zhou","doi":"10.1016/j.gee.2024.01.004","DOIUrl":"https://doi.org/10.1016/j.gee.2024.01.004","url":null,"abstract":"<p>Emerging contaminants (ECs) are widely present in aquatic environments, posing potential risks to both ecosystems and human health. The ultrasound-assisted persulfate oxidation process has attracted considerable attention in the degradation of ECs due to its ability to generate both sulfate radicals and cavitation effects, enhancing degradation effects. In this paper, the principle of ultrasonic synergistic Fenton-like oxidation system for degrading organic pollutants was reviewed, divided into homogeneous system, non-homogeneous system, and single-atom system to explore the synergistic effect of ultrasound-enhanced persulfate technology in three aspects, and the effects of environmental factors such as ultrasonic frequency and power, system pH, temperature, and initial oxidant concentration on the system's decontamination performance were discussed. Finally, future research on ultrasonically activated persulfate technology is summarized and prospected.</p>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"4 1","pages":""},"PeriodicalIF":13.3,"publicationDate":"2024-01-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139465031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}