Green Chemistry最新文献

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Enhanced corrosion resistance of an eco-friendly MXene composite coating with self-healing performance† 具有自修复性能的环保型 MXene 复合涂层的耐腐蚀性能得到增强†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc06219a
Xiaoqing Ma , Tiange Wang , Baolong Gong , Jiale Hou , Shuxian Ji , Huaijie Cao
{"title":"Enhanced corrosion resistance of an eco-friendly MXene composite coating with self-healing performance†","authors":"Xiaoqing Ma ,&nbsp;Tiange Wang ,&nbsp;Baolong Gong ,&nbsp;Jiale Hou ,&nbsp;Shuxian Ji ,&nbsp;Huaijie Cao","doi":"10.1039/d4gc06219a","DOIUrl":"10.1039/d4gc06219a","url":null,"abstract":"<div><div>Though various kinds of self-healing composite coatings have been proposed for long-term corrosion protection of metals toward sustainable development, the construction of highly efficient and thin coatings <em>via</em> an eco-friendly and time-saving process still remains a challenge. Herein, by combining MXene with strong impermeability and tannic acid as a green corrosion inhibitor, a calcium myristate/MXene composite coating was designed for Al alloys. The resultant thin composite coating (∼21.59 μm) exhibited high corrosion resistance, with a decreased corrosion current density of 7.028 × 10<sup>−9</sup> A cm<sup>−2</sup> in a 3.5 wt% NaCl solution, as confirmed by electrochemical tests, surpassing the performances of calcium myristate and calcium myristate/MXene coatings without tannic acid. The self-healing capability was evaluated by electrochemical tests and the evolution of surface morphology of the scratched coating. The damaged MXene composite coating presented self-healing behavior, with a high self-healing efficiency of 99.53% after 8 days. The self-healing mechanism was attributed to the release of tannic acid from the damaged areas. In contrast to the complex functionalization and preparation process of organic coatings, the comprehensive advantages of this MXene composite coating outperformed those of previously reported self-healing MXene coatings. This work provides a facile strategy for constructing self-healing MXene coatings and expands the application potential of MXene.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4369-4384"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826548","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Bio-oil derived polyesteramides as water-degradable replacements for polyethylene† 生物油衍生聚酯酰胺作为聚乙烯† 的水降解替代品
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc05490c
Yohei Yoshinaka , Stephen A. Miller
{"title":"Bio-oil derived polyesteramides as water-degradable replacements for polyethylene†","authors":"Yohei Yoshinaka ,&nbsp;Stephen A. Miller","doi":"10.1039/d4gc05490c","DOIUrl":"10.1039/d4gc05490c","url":null,"abstract":"<div><div>The seed oil from <em>Brassica carinata</em> is a promising source for biobased aviation fuel. Interestingly, the seeds contain considerable sinapic acid and erucic acid, both of which can be utilized for bioplastic synthesis. From the latter, we report herein the synthesis of biobased and water-degradable polyesteramides (PEAs) <em>via N</em>,<em>N</em>′-bis(2-hydroxyethyl)brassylamide (BHEBA). This diol was prepared from ethanolamine and brassylic acid, a C13 oxidation product of the C22 erucic acid, which makes up 42% of the fatty acids present in this non-GMO (non-genetically modified) Ethiopian mustard seed oil. After optimization of conditions, BHEBA was polymerized with aliphatic diacids to obtain the designed PEAs with high purified yields (77–88%) and good molecular weights (<em>M</em><sub>n</sub> = 7000–10 700 Da). The melting temperatures of these PEAs ranged from 130–139 °C, values comparable to those of several grades of polyethylene. Compared to shorter diacids, the brassylic acid incorporated into PEA structures improves hydrophobicity, and mechanical performance was not compromised after a daylong exposure to water. Furthermore, a 12-month PEA degradation study revealed significant hydrolytic degradation (at least 37% loss in <em>M</em><sub>n</sub>) under all the conditions studied: pH 2, pH 5, seawater, and deionized water. Their degradability was further evaluated under high-temperature conditions compared to several commercial plastics, establishing their superior degradability in seawater and deionized water. Chemical recyclability of PEA was demonstrated through facile aminolysis with ethanolamine to regenerate the BHEBA monomer in 84% yield. While further mechanical property improvement would be ideal, the results substantiate the high potential of brassylic acid-based polyesteramides to be eco-friendly replacements for some petroleum-derived commodity plastics, especially polyethylene.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4152-4164"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826530","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Protective fractionation of highly uncondensed lignin with high purity and high yield: new insights into propanediol-blocked lignin condensation†
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d5gc00024f
Yaling Zhao , Deqing Zhao , Jingpeng He , Kaibin Ma , Jiatian Zhu , Jianrong Liu , Yongqi Zhang , Qinqin Xia , Ting Li
{"title":"Protective fractionation of highly uncondensed lignin with high purity and high yield: new insights into propanediol-blocked lignin condensation†","authors":"Yaling Zhao ,&nbsp;Deqing Zhao ,&nbsp;Jingpeng He ,&nbsp;Kaibin Ma ,&nbsp;Jiatian Zhu ,&nbsp;Jianrong Liu ,&nbsp;Yongqi Zhang ,&nbsp;Qinqin Xia ,&nbsp;Ting Li","doi":"10.1039/d5gc00024f","DOIUrl":"10.1039/d5gc00024f","url":null,"abstract":"<div><div>A lignin-first separation strategy can help improve the economic and environmental benefits of biorefinery. However, the self-condensation of lignin remains an insurmountable bottleneck in its isolation and valorization process. Therefore, the challenge of lignin separation is how to achieve a highly uncondensed lignin with high yield and high purity. In this work, we developed a ternary deep eutectic solvent (DES) based on polyhydric alcohols, which can be used to treat moso bamboo at 80–90 °C to obtain highly uncondensed lignin which is light-colored and highly active. The uncondensed lignin exhibits a high β-O-4 retention rate, up to 52.82/100Ar, accounting for 90.24% of the β-O-4 content in the raw material. At the same time, the maximum yield and purity of uncondensed lignin can reach 33.6% and 95.5%, respectively. Furthermore, through DFT theoretical calculations, we have proved that the lignin protection strategy by 1,2-propanediol is achieved by grafting the hydroxyl functional group to the α position of the benzylic carbocation intermediate, thus revealing the intrinsic mechanism by which polyol effectively blocks lignin condensation. The lignin-first fractionation strategy based on ternary deep eutectic solvents with polyhydric alcohols and Lewis acids overcomes the defects of lignin condensation that is inevitable during lignin separation and depolymerization. It obtains highly uncondensed lignin with high yield and high purity, and provides a new idea for biorefinery under the lignin-first separation strategy.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4244-4258"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Tailoring the electronic structure and acid–base properties of MgO by Ce doping promotes biomass-derived formic acid production at room temperature† 通过掺杂 Ce 调整氧化镁的电子结构和酸碱特性,促进生物质甲酸的室温生产†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d5gc00008d
Yiqi Geng , Wenhua Xue , Jian Ye , Ruilong Zhang , Puranjan Mishra , Jun Zhao
{"title":"Tailoring the electronic structure and acid–base properties of MgO by Ce doping promotes biomass-derived formic acid production at room temperature†","authors":"Yiqi Geng ,&nbsp;Wenhua Xue ,&nbsp;Jian Ye ,&nbsp;Ruilong Zhang ,&nbsp;Puranjan Mishra ,&nbsp;Jun Zhao","doi":"10.1039/d5gc00008d","DOIUrl":"10.1039/d5gc00008d","url":null,"abstract":"<div><div>Biomass-based monosaccharide oxidation for formic acid production is significant due to its potential to provide a sustainable, bio-based alternative to traditional fossil fuel-derived methods of formic acid synthesis. In this study, we developed a Ce–MgO catalyst by incorporating Ce to enhance the oxidation of glucose to formic acid. Compared to unmodified MgO, the Ce–MgO catalyst exhibits an increased number of basic sites and higher charge densities at the Mg and O sites. These modifications facilitate the selective dissociation of hydrogen peroxide to form ˙OOH species and enhance the adsorption of ˙OOH at the MgO sites. The electron-rich nature of these Mg(OH)(OOH) active sites lowers the energy barrier for the C–C cleavage and oxidation reaction through more efficient electron transfer. Consequently, the reaction can be conducted at room temperature, achieving a 97.34% conversion of glucose and 93.65% yield of formic acid, which represents the highest performance among all glucose oxidation catalysts for formic acid production. Furthermore, the Ce–MgO catalyst demonstrated its efficacy in catalyzing the oxidation of a mixed sugar solution derived from corncob, achieving a formic acid yield of 49.13% at 30 °C. Additionally, the formic acid produced <em>via</em> this process enables <em>in situ</em> hydrogen production at room temperature, highlighting an effective and sustainable approach for generating green hydrogen from biomass.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4165-4176"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826531","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sustainable and biobased self-blown polycarbonate foams: from synthesis to application† 可持续和生物基自发泡聚碳酸酯泡沫:从合成到应用†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc06429a
Tansu Abbasoglu , Xabier Lopez de Pariza , Gabriel Perli , Danila Merino , Phœbé Caillard-Humeau , Antoine Duval , Luc Avérous , Lourdes Irusta , Alba González , Haritz Sardon
{"title":"Sustainable and biobased self-blown polycarbonate foams: from synthesis to application†","authors":"Tansu Abbasoglu ,&nbsp;Xabier Lopez de Pariza ,&nbsp;Gabriel Perli ,&nbsp;Danila Merino ,&nbsp;Phœbé Caillard-Humeau ,&nbsp;Antoine Duval ,&nbsp;Luc Avérous ,&nbsp;Lourdes Irusta ,&nbsp;Alba González ,&nbsp;Haritz Sardon","doi":"10.1039/d4gc06429a","DOIUrl":"10.1039/d4gc06429a","url":null,"abstract":"<div><div>Escalating environmental concerns driven by the continuous demand for fossil-based materials have sparked growing interest in designing biobased polymeric materials for high-added-value applications. A novel series of self-blowing polycarbonate foams derived from various biobased polyols (<em>e.g.</em> cashew nutshell liquid, vegetable oil, and lignocellulose) is reported by leveraging thiol-triggered carbon dioxide release in a formulation composed of a thiol and 5- and 6-membered cyclic carbonates. The polyol architecture enabled a tunable open-cell morphology and properties, achieving up to 41 wt% biobased content, marking the first incorporation of biobased monomers in this type of foam. In this context, cashew nutshell-based foam featured good cyclic endurance at 70% compression and a high-water uptake capacity of 8 g g<sup>−1</sup>. As a forward-looking solution to address environmental challenges, this foam effectively supports the germination of different types of vegetable seeds (<em>e.g.</em> bok choy (<em>Brassica rapa chinensis</em>), lettuce (<em>Lactuca sativa</em>), and radish (<em>Raphanus sativus</em>)) in soilless environments, and its hydrolytic stability ensures reusability for subsequent seedling growth. This study lays the foundation for designing future environmentally friendly and renewable polymeric foams that are potentially recyclable with sustainable applications, <em>e.g.</em>, in hydroponics.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4341-4351"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826546","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Water-assisted clean electro-preparation of Co3Fe7 in molten salts: its enhanced ferromagnetic properties and hydrogen evolution rate† 水辅助清洁电制备熔盐中的 Co3Fe7:增强的铁磁特性和氢进化率†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc05961a
Shengxi Zhao , Kaiyu Xie , Ali Reza Kamali
{"title":"Water-assisted clean electro-preparation of Co3Fe7 in molten salts: its enhanced ferromagnetic properties and hydrogen evolution rate†","authors":"Shengxi Zhao ,&nbsp;Kaiyu Xie ,&nbsp;Ali Reza Kamali","doi":"10.1039/d4gc05961a","DOIUrl":"10.1039/d4gc05961a","url":null,"abstract":"<div><div>A clean and efficient method for synthesizing intermetallic Co<sub>3</sub>Fe<sub>7</sub> is reported, based on water-assisted molten salt electrolysis employing the CoFe<sub>2</sub>O<sub>4</sub> electrode, fabricated through the thermo-mechanochemical treatment of iron and cobalt oxides. The electrolysis is conducted at a cell voltage of 1.5 V, achieving an energy consumption of 1.47 kW h kg<sup>−1</sup>. Upon formation, the synthesized Co<sub>3</sub>Fe<sub>7</sub> serves as an electrode for catalytic hydrogen production, demonstrating a current density of 91.7 mA cm<sup>−2</sup>. These performances are compared with those of electrolytic Fe (1.49 kW h kg<sup>−1</sup> and 96.4 mA cm<sup>−2</sup>) and electrolytic Co (1.30 kW h kg<sup>−1</sup> and 40.8 mA cm<sup>−2</sup>), both prepared under the same electrolysis potential but with different current–time profiles. The electrolytic Co<sub>3</sub>Fe<sub>7</sub> exhibits superior ferromagnetic properties, with saturation magnetization, remanent magnetization and coercivity values of 157.0 emu g<sup>−1</sup>, 4.3 emu g<sup>−1</sup> and 48.9 Oe, respectively, surpassing values reported in the literature for Fe–Co alloys. The findings suggest a sustainable approach for the green synthesis of Co<sub>3</sub>Fe<sub>7</sub> with enhanced ferromagnetic properties. Additionally, the electrolytic Fe and Co<sub>3</sub>Fe<sub>7</sub> show promise as electrode materials for molten salt hydrogen production.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4320-4329"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826544","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Sustainable lithium recovery from geothermal brine via integrated membrane distillation – selective electrodialysis 通过集成膜蒸馏-选择性电渗析从地热卤水中进行可持续的锂回收
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc06530a
Roviel Berhane Zegeye , Ramato Ashu Tufa , Sergio Santoro , Bruno Marco Inzillo , Marco Aquino , Grazia Giuseppina Politano , Alula Selomon Embaye , Pietro Argurio , Loredana De Bartolo , Efrem Curcio
{"title":"Sustainable lithium recovery from geothermal brine via integrated membrane distillation – selective electrodialysis","authors":"Roviel Berhane Zegeye ,&nbsp;Ramato Ashu Tufa ,&nbsp;Sergio Santoro ,&nbsp;Bruno Marco Inzillo ,&nbsp;Marco Aquino ,&nbsp;Grazia Giuseppina Politano ,&nbsp;Alula Selomon Embaye ,&nbsp;Pietro Argurio ,&nbsp;Loredana De Bartolo ,&nbsp;Efrem Curcio","doi":"10.1039/d4gc06530a","DOIUrl":"10.1039/d4gc06530a","url":null,"abstract":"<div><div>The escalating global demand for lithium, driven by its crucial role in energy storage systems and the transition to renewable energy, necessitates sustainable extraction methods from innovative sources such as geothermal brines, salt lakes and recycled batteries. Geothermal brine offers a dual advantage as a source of clean energy and lithium, with higher lithium concentrations (0.01–0.48 g L<sup>−1</sup>) compared to seawater (0.18 mg L<sup>−1</sup>) and levels comparable to salt lakes (0.04–3 g L<sup>−1</sup>). Additionally, it features a much lower Mg/Li ratio (∼35.33) compared to seawater (∼7588), though still higher than that of salt lakes (∼6.4). Despite these advantages, lithium recovery from geothermal brines is challenging due to low lithium concentrations and the presence of competing ions. Herein, we introduce a novel approach that integrates Membrane Distillation (MD) and Selective Electrodialysis (S-ED) for efficient lithium extraction and water recovery from geothermal brines. The focus is on optimizing performance at both stages: The MD process was optimized to reduce brine volume and specific thermal energy consumption, while the ED process was focused on minimizing voltage and specific energy consumption at the optimal concentration. The hybrid system demonstrates strong potential for energy-efficient lithium recovery. At MD stage, geothermal water was concentrated at different volume reduction factors (VRFs) of 15.1, 28.1 and 43.11, resulting in feed concentrations of 1 M, 2 M, and 3 M, respectively, for the subsequent ED stage. Operating the MD process with geothermal water at its natural temperature of 40 °C rendered it energy-neutral, leading to specific thermal energy savings of up to 1980.5 kW h m<sup>−3</sup>. At S-ED stage, higher feed concentrations improved lithium selectivity but increased specific energy consumption. The optimal performance was observed at a feed concentration of 2 M (corresponding MD-VRF of 28.1) and an applied voltage of 2 V, achieving a specific energy consumption of 0.04 kW h per gram of Li<sup>+</sup> and a current efficiency of 4.1%. Overall, the integrated MD–S-ED approach demonstrates strong potential for energy-efficient lithium recovery, paving the way for innovative research and offering key insights for sustainable lithium extraction methods that support the principle of Circular Blue Economy and Green Process Intensification.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4205-4221"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826534","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Electrochemical α-hydroxylation of aryl ketones with methanol as the oxygen source† 以甲醇为氧源进行芳基酮的电化学α-羟基化反应†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d5gc00758e
Zhaoliang Yang , Jianwei Huang , Yahao Wang , Haiyan Du , Yuan Zhou , Mingming Yu
{"title":"Electrochemical α-hydroxylation of aryl ketones with methanol as the oxygen source†","authors":"Zhaoliang Yang ,&nbsp;Jianwei Huang ,&nbsp;Yahao Wang ,&nbsp;Haiyan Du ,&nbsp;Yuan Zhou ,&nbsp;Mingming Yu","doi":"10.1039/d5gc00758e","DOIUrl":"10.1039/d5gc00758e","url":null,"abstract":"<div><div>Selective hydroxylation of Csp<sup>3</sup>–H bonds is challenging but highly valuable. This report describes electrochemical α-hydroxylation of aryl ketones under mild conditions without transition metal catalysts or oxygen gas; methanol serves as the oxygen source for preparing a series of compounds. Using deuterated methanol leads to α-deuterohydroxylation in a single step, thus offering a convenient isotope labeling approach. This method can be applied to effectively hydroxylate secondary Csp<sup>3</sup>–H bonds. Mechanistic investigations confirm methanol as the oxygen source, and scale-up experiments highlight the practical applicability of this reaction.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4128-4133"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826527","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enhancing the selectivity of C2 hydrocarbons over Fe-based catalysts by controlling nitrogen doping in electrocatalytic CO2 reduction†
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d5gc00678c
Peng Chen , Shiqiang Liu , Pei Zhang , Xinchen Kang , Xing Tong , Jun Ma , Chunjun Chen , Zhimin Liu , Xueqing Xing , Zhonghua Wu , Lirong Zheng , Buxing Han
{"title":"Enhancing the selectivity of C2 hydrocarbons over Fe-based catalysts by controlling nitrogen doping in electrocatalytic CO2 reduction†","authors":"Peng Chen ,&nbsp;Shiqiang Liu ,&nbsp;Pei Zhang ,&nbsp;Xinchen Kang ,&nbsp;Xing Tong ,&nbsp;Jun Ma ,&nbsp;Chunjun Chen ,&nbsp;Zhimin Liu ,&nbsp;Xueqing Xing ,&nbsp;Zhonghua Wu ,&nbsp;Lirong Zheng ,&nbsp;Buxing Han","doi":"10.1039/d5gc00678c","DOIUrl":"10.1039/d5gc00678c","url":null,"abstract":"<div><div>Rational design of cost-effective materials as highly efficient catalysts for the electrochemical CO<sub>2</sub> reduction reaction (CO<sub>2</sub>RR) to produce multi-carbon (C<sub>2+</sub>) hydrocarbons is highly desirable. Cu-based catalysts are widely recognized as effective for the electrosynthesis of multi-carbon products. Exploration of non-copper-based catalysts for C<sub>2+</sub> products is very interesting and challenging. In this work, using ethylenediaminetetraacetic acid disodium salt and ethylenediamine as the ligands and N source, N-doped Fe<sub>2</sub>O<sub>3</sub> catalysts containing FeO<sub>1−<em>x</em></sub>N<sub><em>x</em></sub> (0.34 &lt; <em>x</em> &lt; 0.54) sites with and without a FeN<sub>4</sub> structure were fabricated. It was found that the catalyst without a FeN<sub>4</sub> structure converted CO<sub>2</sub> to C<sub>2</sub> hydrocarbons (ethane and ethylene). The faradaic efficiency (FE) of C<sub>2</sub> products and the current density of C<sub>2</sub> products reached 60.8% and 39.1 mA cm<sup>−2</sup>, respectively, which is currently the best result for non-copper catalysts in an H-cell. However, the FE of the catalyst with a FeN<sub>4</sub> structure was much lower when producing C<sub>2</sub> products. Detailed study showed that the FeO<sub>1−<em>x</em></sub>N<sub><em>x</em></sub> sites with suitable coordination of N with Fe was pivotal to the high FE of C<sub>2</sub> products. A combination of experimental and density functional theory studies indicated that the feasible coordination of N with Fe resulted in the deformation of the electron cloud around the Fe nucleus, which facilitated the charge transfer and promoted the production of C<sub>2</sub> products. This work provides a successful example of designing non-copper catalysts for producing C<sub>2+</sub> products in the CO<sub>2</sub>RR.</div></div>","PeriodicalId":78,"journal":{"name":"Green Chemistry","volume":"27 16","pages":"Pages 4134-4142"},"PeriodicalIF":9.3,"publicationDate":"2025-03-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143826528","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
On the use of propylene carbonate and dimethyl carbonate as green solvents in organic electrosynthesis† 论碳酸丙烯酯和碳酸二甲酯作为绿色溶剂在有机电合成中的应用†。
IF 9.3 1区 化学
Green Chemistry Pub Date : 2025-03-05 DOI: 10.1039/d4gc06199c
Adrian Prudlik , Alexandra Matei , Anton Scherkus , Javier Ivan Bardagi , Sebastian B. Beil , Robert Francke
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