Emerging excessive greenhouse gas emissions pose great threats to the ecosystem, which thus requires efficient CO2 capture to mitigate the disastrous issue. In this report, large molecular size bisphenol A ethoxylate diacrylate (BPA) was employed to crosslink poly (ethylene glycol) methyl ether acrylate (PEGMEA) via the green and rapid UV polymerization strategy. The microstructure of such-prepared membrane could be conveniently tailored by tuning the ratio of the two prepolymers, aiming at obtaining the optimized microstructures with suitable mesh size and PEO sol content, which was approved by a novel low-field nuclear magnetic resonance technique. The optimum membrane overcomes the trade-off challenge: dense microstructures lower the gas permeability while loose microstructures lower high-pressure-resistance capacity, realizing a high CO2 permeability of 1711 Barrer and 100-h long-term running stability under 15 atm. The proposed membrane fabrication approach, hence, opens a novel gate for developing high-performance robust membranes for CO2 capture.
{"title":"Tailor-made microstructures lead to high-performance robust PEO membrane for CO2 capture via green fabrication technique","authors":"Wei-Shi Sun, Ming-Jie Yin, Wen-Hai Zhang, Shuo Li, Naixin Wang, Quan-Fu An","doi":"10.1016/j.gee.2022.01.016","DOIUrl":"https://doi.org/10.1016/j.gee.2022.01.016","url":null,"abstract":"<div><p>Emerging excessive greenhouse gas emissions pose great threats to the ecosystem, which thus requires efficient CO<sub>2</sub> capture to mitigate the disastrous issue. In this report, large molecular size bisphenol A ethoxylate diacrylate (BPA) was employed to crosslink poly (ethylene glycol) methyl ether acrylate (PEGMEA) via the green and rapid UV polymerization strategy. The microstructure of such-prepared membrane could be conveniently tailored by tuning the ratio of the two prepolymers, aiming at obtaining the optimized microstructures with suitable mesh size and PEO sol content, which was approved by a novel low-field nuclear magnetic resonance technique. The optimum membrane overcomes the trade-off challenge: dense microstructures lower the gas permeability while loose microstructures lower high-pressure-resistance capacity, realizing a high CO<sub>2</sub> permeability of 1711 Barrer and 100-h long-term running stability under 15 atm. The proposed membrane fabrication approach, hence, opens a novel gate for developing high-performance robust membranes for CO<sub>2</sub> capture.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1389-1397"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175618","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 : 2023-10-01DOI: 10.1016/j.gee.2022.02.009
Yuxin Gao , Jiang Zhou , Liping Qin , Zhenming Xu , Zhexuan Liu , Liangbing Wang , Xinxin Cao , Guozhao Fang , Shuquan Liang
Rapid capacity decay and sluggish reaction kinetics are major barriers hindering the applications of manganese-based cathode materials for aqueous zinc-ion batteries. Herein, the effects of crystal plane on the in-situ transformation behavior and electrochemical performance of manganese-based cathode is discussed. A comprehensive discussion manifests that the exposed (100) crystal plane is beneficial to the phase transformation from tunnel-structured MnO2 to layer-structured ZnMn3O7·3H2O, which plays a critical role for the high reactivity, high capacity, fast diffusion kinetics and long cycling stability. Additionally, a two-stage zinc storage mechanism can be demonstrated, involving continuous activation reaction and phase transition reaction. As expected, it exhibits a high capacity of 275 mAh g−1 at 100 mA g−1, a superior durability over 1000 cycles and good rate capability. This study may open new windows toward developing advanced cathodes for ZIBs, and facilitate the applications of ZIBs in large-scale energy storage system.
快速的容量衰减和缓慢的反应动力学是阻碍锰基阴极材料在水性锌离子电池中应用的主要障碍。本文讨论了晶面对锰基阴极原位转化行为和电化学性能的影响。综合讨论表明,暴露的(100)晶面有利于从隧道结构的MnO2向层结构的ZnMn3O7·3H2O的相变,这对高反应性、高容量、快速扩散动力学和长循环稳定性起着关键作用。此外,还可以证明锌的两阶段储存机制,包括连续活化反应和相变反应。正如预期的那样,它在100 mA g−1下表现出275 mAh g−1的高容量,在1000次循环中具有卓越的耐用性和良好的倍率性能。这项研究可能为开发先进的ZIBs阴极打开新的窗口,并促进ZIBs在大规模储能系统中的应用。
{"title":"Crystal plane induced in-situ electrochemical activation of manganese-based cathode enable long-term aqueous zinc-ion batteries","authors":"Yuxin Gao , Jiang Zhou , Liping Qin , Zhenming Xu , Zhexuan Liu , Liangbing Wang , Xinxin Cao , Guozhao Fang , Shuquan Liang","doi":"10.1016/j.gee.2022.02.009","DOIUrl":"https://doi.org/10.1016/j.gee.2022.02.009","url":null,"abstract":"<div><p>Rapid capacity decay and sluggish reaction kinetics are major barriers hindering the applications of manganese-based cathode materials for aqueous zinc-ion batteries. Herein, the effects of crystal plane on the <em>in-situ</em> transformation behavior and electrochemical performance of manganese-based cathode is discussed. A comprehensive discussion manifests that the exposed (100) crystal plane is beneficial to the phase transformation from tunnel-structured MnO<sub>2</sub> to layer-structured ZnMn<sub>3</sub>O<sub>7</sub>·3H<sub>2</sub>O, which plays a critical role for the high reactivity, high capacity, fast diffusion kinetics and long cycling stability. Additionally, a two-stage zinc storage mechanism can be demonstrated, involving continuous activation reaction and phase transition reaction. As expected, it exhibits a high capacity of 275 mAh g<sup>−1</sup> at 100 mA g<sup>−1</sup>, a superior durability over 1000 cycles and good rate capability. This study may open new windows toward developing advanced cathodes for ZIBs, and facilitate the applications of ZIBs in large-scale energy storage system.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1429-1436"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175645","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}
Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications, such as the electrodes of supercapacitors; however, the improvement of their energy density remains a challenge. Here, we design a green and universal approach to prepare the composite electrode material, which is composed of lignin-phenol-formaldehyde resins derived hierarchical porous carbon (LR-HPC) as conductive skeletons and the self-assembly manganese cobaltite (MnCo2O4) nanocrystals as active sites. The synthesized C@MnCo2O4 composite has an abundant porous structure and superior electronic conductivity, allowing for more charge/electron mass transfer channels and active sites for the redox reactions. The composite shows excellent electrochemical performance, such as the maximum specific capacitance of ∼726 mF cm−2 at 0.5 mV s−1, due to the significantly enhanced interactive interface between LR-HPC and MnCo2O4 crystals. The assembled all-solid-state asymmetric supercapacitor, with the LR-HPC and C@MnCo2O4 as cathode and anode, respectively, exhibits the highest volumetric energy density of 0.68 mWh cm−3 at a power density of 8.2 mW cm−3. Moreover, this device shows a high capacity retention ratio of ∼87.6% at 5 mA cm−2 after 5000 cycles.
{"title":"Efficient conversion of lignin waste and self-assembly synthesis of C@MnCo2O4 for asymmetric supercapacitors with high energy density","authors":"Jiahui Mu, Cuihuan Li, Jiankang Zhang, Xianliang Song, Sheng Chen, Feng Xu","doi":"10.1016/j.gee.2022.09.010","DOIUrl":"https://doi.org/10.1016/j.gee.2022.09.010","url":null,"abstract":"<div><p>Lignin waste from the papermaking and biorefineries industry is a significantly promising renewable resource to prepare advanced carbon materials for diverse applications, such as the electrodes of supercapacitors; however, the improvement of their energy density remains a challenge. Here, we design a green and universal approach to prepare the composite electrode material, which is composed of lignin-phenol-formaldehyde resins derived hierarchical porous carbon (LR-HPC) as conductive skeletons and the self-assembly manganese cobaltite (MnCo<sub>2</sub>O<sub>4</sub>) nanocrystals as active sites. The synthesized C@MnCo<sub>2</sub>O<sub>4</sub> composite has an abundant porous structure and superior electronic conductivity, allowing for more charge/electron mass transfer channels and active sites for the redox reactions. The composite shows excellent electrochemical performance, such as the maximum specific capacitance of ∼726 mF cm<sup>−2</sup> at 0.5 mV s<sup>−1</sup>, due to the significantly enhanced interactive interface between LR-HPC and MnCo<sub>2</sub>O<sub>4</sub> crystals. The assembled all-solid-state asymmetric supercapacitor, with the LR-HPC and C@MnCo<sub>2</sub>O<sub>4</sub> as cathode and anode, respectively, exhibits the highest volumetric energy density of 0.68 mWh cm<sup>−3</sup> at a power density of 8.2 mW cm<sup>−3</sup>. Moreover, this device shows a high capacity retention ratio of ∼87.6% at 5 mA cm<sup>−2</sup> after 5000 cycles.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1479-1487"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175650","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 : 2023-10-01DOI: 10.1016/j.gee.2022.06.008
Pingping Yang , Xin Yang , Wenzhu Liu , Ruike Guo , Zufu Yao
Graphene-based nanocatalysts have appealed much interest as advanced electrocatalysts toward energy conversion reactions due to their outstanding electrocatalytic performance from the distinctive chemical composites and strong synergistic effects. Aiming to better understand the role of graphene played in enhancing the catalytic performance and offer guidance for fabricating more efficient graphene-based electrocatalysts, we herein summarize the remarkable achievements of graphene-based electrocatalysts for energy-conversion-related reactions. Started by discussing applications of graphene in the electrocatalytic reactions, we have manifested the crucial role of graphene played in promoting the catalytic performance. Subsequently, many representative graphene-based catalyst hybrids for electrocatalytic reactions are also overviewed, showing many effective strategies for the fabrication of more efficient graphene-related materials for the practical application. Finally, the perspective insights and challenging issues are also concluded to provide directions for the future development.
{"title":"Graphene-based electrocatalysts for advanced energy conversion","authors":"Pingping Yang , Xin Yang , Wenzhu Liu , Ruike Guo , Zufu Yao","doi":"10.1016/j.gee.2022.06.008","DOIUrl":"https://doi.org/10.1016/j.gee.2022.06.008","url":null,"abstract":"<div><p>Graphene-based nanocatalysts have appealed much interest as advanced electrocatalysts toward energy conversion reactions due to their outstanding electrocatalytic performance from the distinctive chemical composites and strong synergistic effects. Aiming to better understand the role of graphene played in enhancing the catalytic performance and offer guidance for fabricating more efficient graphene-based electrocatalysts, we herein summarize the remarkable achievements of graphene-based electrocatalysts for energy-conversion-related reactions. Started by discussing applications of graphene in the electrocatalytic reactions, we have manifested the crucial role of graphene played in promoting the catalytic performance. Subsequently, many representative graphene-based catalyst hybrids for electrocatalytic reactions are also overviewed, showing many effective strategies for the fabrication of more efficient graphene-related materials for the practical application. Finally, the perspective insights and challenging issues are also concluded to provide directions for the future development.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1265-1278"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175611","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 : 2023-10-01DOI: 10.1016/j.gee.2022.02.001
Ruixiang Qu , Shuaiheng Zhao , Na Liu , Xiangyu Li , Huajun Zhai , Ya'nan Liu , Yen Wei , Lin Feng
Although oily wastewater treatment realized by superwetting materials has attracted heightened attention in recent years, how to treat enormous-volume emulsion wastewater is still a tough problem, which is ascribed to the emulsion accumulation. Herein, to address this problem, a material is presented by subtly integrating chemical demulsification and 3D inner-outer asymmetric wettability to a sponge substrate, and thus wettability gradient-driven oil directional transport for achieving unprecedented enormous-volume emulsion wastewater treatment is realized based on a “demulsification-transport” mechanism. The maximum treatment volume realized by the sponge is as large as 3 L (2.08 × 104 L per cubic meter of the sponge) in one cycle, which is about 100 times of the reported materials. Besides, owing to the large pore size of the sponge, 9000 L m2 h−1 (LMH) separation flux and 99.5% separation efficiency are realized simultaneously, which overcomes the trade-off dilemma. Such a 3D inner-outer asymmetric sponge displaying unprecedented advantage in the treatment volume can promote the development of the oily wastewater treatment field, as well as expand the application prospects of superwetting materials, especially in continuous water treatment.
尽管近年来超润湿材料处理含油废水引起了人们的高度重视,但如何处理大体积乳化废水仍然是一个难题,这归因于乳化液的积累。在此,为了解决这个问题,提出了一种将化学破乳和三维内外不对称润湿性巧妙地结合到海绵基底上的材料,从而基于“破乳传输”机制实现了润湿性梯度驱动的油定向传输,以实现前所未有的大体积乳化废水处理。海绵在一个循环中实现的最大处理量高达3L(每立方米海绵2.08×104L),约为报道材料的100倍。此外,由于海绵的孔径较大,同时实现了9000 L m2 h−1(LMH)的分离通量和99.5%的分离效率,克服了折衷的困境。这种三维内外不对称海绵在处理体积上显示出前所未有的优势,可以促进含油废水处理领域的发展,并拓展超润湿材料的应用前景,特别是在连续水处理中。
{"title":"3D inner-outer asymmetric sponge for enormous-volume emulsion wastewater treatment based on a new “demulsification-transport” mechanism","authors":"Ruixiang Qu , Shuaiheng Zhao , Na Liu , Xiangyu Li , Huajun Zhai , Ya'nan Liu , Yen Wei , Lin Feng","doi":"10.1016/j.gee.2022.02.001","DOIUrl":"https://doi.org/10.1016/j.gee.2022.02.001","url":null,"abstract":"<div><p>Although oily wastewater treatment realized by superwetting materials has attracted heightened attention in recent years, how to treat enormous-volume emulsion wastewater is still a tough problem, which is ascribed to the emulsion accumulation. Herein, to address this problem, a material is presented by subtly integrating chemical demulsification and 3D inner-outer asymmetric wettability to a sponge substrate, and thus wettability gradient-driven oil directional transport for achieving unprecedented enormous-volume emulsion wastewater treatment is realized based on a “demulsification-transport” mechanism. The maximum treatment volume realized by the sponge is as large as 3 L (2.08 × 10<sup>4</sup> L per cubic meter of the sponge) in one cycle, which is about 100 times of the reported materials. Besides, owing to the large pore size of the sponge, 9000 L m<sup>2</sup> h<sup>−1</sup> (LMH) separation flux and 99.5% separation efficiency are realized simultaneously, which overcomes the trade-off dilemma. Such a 3D inner-outer asymmetric sponge displaying unprecedented advantage in the treatment volume can promote the development of the oily wastewater treatment field, as well as expand the application prospects of superwetting materials, especially in continuous water treatment.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1398-1408"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175614","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 : 2023-10-01DOI: 10.1016/j.gee.2022.02.008
Jiamiao Ran , Hui Liu , Hongliang Dong , Peng Gao , Haowei Cheng , Jianing Xu , Hailun Wang , Zixing Wang , Qingfeng Fu , Jiaxu Yan , Jilei Liu
Bronze phase titanium dioxide (TiO2(B)) could be a promising high-power anode for lithium ion battery. However, TiO2(B) is a metastable material, so the as-synthesized samples are inevitably accompanied by the existence of anatase phases. It has been found that the TiO2(B)'s purity is positively correlated with its electrochemical performance. Herein, we have established an accurate quantification of the TiO2(B)/anatase ratio, by figuring out the function between the purity of TiO2(B) phase in the high purity range and its Raman spectra features in combination of the calibration by the synchrotron radiation X-ray diffraction (XRD). Compared with the time-consuming electrochemical method, the rapid, sensitive and non-destructive features of Raman spectroscopy have made it a promising candidate for determining the purity of TiO2(B). Further, the correlations developed in this work should be instructive in synthesizing pure TiO2(B) and furthermore optimizing its electrochemical charge storage properties.
{"title":"Accurate quantification of TiO2(B)'s phase purity via Raman spectroscopy","authors":"Jiamiao Ran , Hui Liu , Hongliang Dong , Peng Gao , Haowei Cheng , Jianing Xu , Hailun Wang , Zixing Wang , Qingfeng Fu , Jiaxu Yan , Jilei Liu","doi":"10.1016/j.gee.2022.02.008","DOIUrl":"https://doi.org/10.1016/j.gee.2022.02.008","url":null,"abstract":"<div><p>Bronze phase titanium dioxide (TiO<sub>2</sub>(B)) could be a promising high-power anode for lithium ion battery. However, TiO<sub>2</sub>(B) is a metastable material, so the as-synthesized samples are inevitably accompanied by the existence of anatase phases. It has been found that the TiO<sub>2</sub>(B)'s purity is positively correlated with its electrochemical performance. Herein, we have established an accurate quantification of the TiO<sub>2</sub>(B)/anatase ratio, by figuring out the function between the purity of TiO<sub>2</sub>(B) phase in the high purity range and its Raman spectra features in combination of the calibration by the synchrotron radiation X-ray diffraction (XRD). Compared with the time-consuming electrochemical method, the rapid, sensitive and non-destructive features of Raman spectroscopy have made it a promising candidate for determining the purity of TiO<sub>2</sub>(B). Further, the correlations developed in this work should be instructive in synthesizing pure TiO<sub>2</sub>(B) and furthermore optimizing its electrochemical charge storage properties.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 5","pages":"Pages 1371-1379"},"PeriodicalIF":13.3,"publicationDate":"2023-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175716","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}
Clean and efficient recycling of spent lithium-ion batteries (LIBs) has become an urgent need to promote sustainable and rapid development of human society. Therefore, we provide a critical and comprehensive overview of the various technologies for recycling spent LIBs, starting with lithium-ion power batteries. Recent research on raw material collection, metallurgical recovery, separation and purification is highlighted, particularly in terms of all aspects of economic efficiency, energy consumption, technology transformation and policy management. Mechanisms and pathways for transformative full-component recovery of spent LIBs are explored, revealing a clean and efficient closed-loop recovery mechanism. Optimization methods are proposed for future recycling technologies, with a focus on how future research directions can be industrialized. Ultimately, based on life-cycle assessment, the challenges of future recycling are revealed from the LIBs supply chain and stability of the supply chain of the new energy battery industry to provide an outlook on clean and efficient short process recycling technologies. This work is designed to support the sustainable development of the new energy power industry, to help meet the needs of global decarbonization strategies and to respond to the major needs of industrialized recycling.
{"title":"Development of Sustainable and Efficient Recycling Technology for Spent Li-Ion Batteries: Traditional and Transformation Go Hand in Hand","authors":"Zejian Liu, Gongqi Liu, Leilei Cheng, Jing Gu, Haoran Yuan, Yong Chen, Yufeng Wu","doi":"10.1016/j.gee.2023.09.001","DOIUrl":"https://doi.org/10.1016/j.gee.2023.09.001","url":null,"abstract":"Clean and efficient recycling of spent lithium-ion batteries (LIBs) has become an urgent need to promote sustainable and rapid development of human society. Therefore, we provide a critical and comprehensive overview of the various technologies for recycling spent LIBs, starting with lithium-ion power batteries. Recent research on raw material collection, metallurgical recovery, separation and purification is highlighted, particularly in terms of all aspects of economic efficiency, energy consumption, technology transformation and policy management. Mechanisms and pathways for transformative full-component recovery of spent LIBs are explored, revealing a clean and efficient closed-loop recovery mechanism. Optimization methods are proposed for future recycling technologies, with a focus on how future research directions can be industrialized. Ultimately, based on life-cycle assessment, the challenges of future recycling are revealed from the LIBs supply chain and stability of the supply chain of the new energy battery industry to provide an outlook on clean and efficient short process recycling technologies. This work is designed to support the sustainable development of the new energy power industry, to help meet the needs of global decarbonization strategies and to respond to the major needs of industrialized recycling.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"60 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"134995409","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 : 2023-09-01DOI: 10.1016/j.gee.2023.09.002
Yisen Yang, Zhonghao Tan, Jianling Zhang, Jie Yang, Renjie Zhang, Sha Wang, Yi Song, Zhuizhui Su
To improve the electrocatalytic transformation of carbon dioxide (CO2) to multi-carbon (C2+) products is of great importance. Here we developed a nitrogen-doped Cu catalyst, by which the maximum C2+ Faradaic efficiency can reach 72.7% in flow-cell system, with the partial current density reaching 0.62 A cm-2. The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst, thus promoting the *CO utilization in the subsequent C-C coupling step. Simultaneously, the water activation can be well enhanced by N doping on Cu catalyst. Owing to the synergystic effects, the selectivity and activity for C2+ products over the N-deoped Cu catalyst are much improved.
改进二氧化碳(CO2)电催化转化为多碳(C2+)产物具有重要意义。本文研制了一种氮掺杂Cu催化剂,该催化剂在流电池体系中C2+法拉第效率最高可达72.7%,分电流密度可达0.62 a cm-2。原位拉曼光谱表明,n掺杂Cu催化剂对*CO的吸附增强,从而促进了后续C-C耦合步骤中*CO的利用。同时,在Cu催化剂上掺杂N可以很好地增强水活化。由于协同作用,n - Cu催化剂对C2+产物的选择性和活性大大提高。
{"title":"Nitrogen-doping boosts *CO utilization and H2O activation on copper for improving CO2 reduction to C2+ products","authors":"Yisen Yang, Zhonghao Tan, Jianling Zhang, Jie Yang, Renjie Zhang, Sha Wang, Yi Song, Zhuizhui Su","doi":"10.1016/j.gee.2023.09.002","DOIUrl":"https://doi.org/10.1016/j.gee.2023.09.002","url":null,"abstract":"To improve the electrocatalytic transformation of carbon dioxide (CO2) to multi-carbon (C2+) products is of great importance. Here we developed a nitrogen-doped Cu catalyst, by which the maximum C2+ Faradaic efficiency can reach 72.7% in flow-cell system, with the partial current density reaching 0.62 A cm-2. The in situ Raman spectra demonstrate that the *CO adsorption can be strengthened on such a N-doped Cu catalyst, thus promoting the *CO utilization in the subsequent C-C coupling step. Simultaneously, the water activation can be well enhanced by N doping on Cu catalyst. Owing to the synergystic effects, the selectivity and activity for C2+ products over the N-deoped Cu catalyst are much improved.","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"11 1","pages":"0"},"PeriodicalIF":0.0,"publicationDate":"2023-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"135588302","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 : 2023-08-01DOI: 10.1016/j.gee.2021.12.002
Guolang Zhou , Linlin Chen , Xiaowei Li , Guiling Luo , Zhendong Yu , Jingzhou Yin , Lei Fan , Yanhong Chao , Lei Jiang , Wenshuai Zhu
The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn2O4-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn2O4 that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn2O4 (Tr-oh LMO) in which the dominant (111) facets minimize Mn dissolution while a small portion of (100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity (20.25 mg g−1 per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn2O4 in electrochemical lithium recovery.
{"title":"Construction of truncated-octahedral LiMn2O4 for battery-like electrochemical lithium recovery from brine","authors":"Guolang Zhou , Linlin Chen , Xiaowei Li , Guiling Luo , Zhendong Yu , Jingzhou Yin , Lei Fan , Yanhong Chao , Lei Jiang , Wenshuai Zhu","doi":"10.1016/j.gee.2021.12.002","DOIUrl":"https://doi.org/10.1016/j.gee.2021.12.002","url":null,"abstract":"<div><p>The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn<sub>2</sub>O<sub>4</sub>-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn<sub>2</sub>O<sub>4</sub> that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn<sub>2</sub>O<sub>4</sub> (Tr-oh LMO) in which the dominant (111) facets minimize Mn dissolution while a small portion of (100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity (20.25 mg g<sup>−1</sup> per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn<sub>2</sub>O<sub>4</sub> in electrochemical lithium recovery.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 4","pages":"Pages 1081-1090"},"PeriodicalIF":13.3,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175345","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 : 2023-08-01DOI: 10.1016/j.gee.2022.01.011
Daqiang Yan, Lin Zhang, Lei Shen, Runyu Hu, Weiping Xiao, Xiaofei Yang
Developing high efficient Pd-based electrocatalysts for oxygen reduction reaction (ORR) is still challenging for alkaline membrane fuel cell, since the strong oxygen adsorption energy and easy agglomerative intrinsic properties. In order to simultaneously solve these problems, Pd/Co3O4–N–C multidimensional materials with porous structures is designed as the ORR catalysts. In details, the ZIF-67 with polyhedral structure was firstly synthesized and then annealed at high-temperature to prepare the N-doped Co3O4 carbon-based material, which was used to homogeneously confine Pd nanoparticles and obtained the Pd/Co3O4–N–C series catalysts. The formation of Co–N and C–N bond could provide efficient active sites for ORR. Simultaneously, the strong electronic interaction in the interface between the Pd and N-doped Co3O4 could disperse and avoid the agglomeration of Pd nanoparticles and ensure the exposure of active sites, which is crucial to lower the energy barrier toward ORR and substantially enhance the ORR kinetics. Hence, the Pd/Co3O4–N–C nanocompounds exhibited excellent ORR catalytic performance, ideal Pd mass activity, and durability in 0.1 mol L−1 KOH solution compared with Co3O4–N–C and Pd/C. The scalable synthesis method, relatively low cost, and excellent electrochemical ORR performance indicated that the obtained Pd/Co3O4–N–C electrocatalyst had the potential for application on fuel cells.
{"title":"Pd nanoparticles embedded in N-Enriched MOF-Derived architectures for efficient oxygen reduction reaction in alkaline media","authors":"Daqiang Yan, Lin Zhang, Lei Shen, Runyu Hu, Weiping Xiao, Xiaofei Yang","doi":"10.1016/j.gee.2022.01.011","DOIUrl":"https://doi.org/10.1016/j.gee.2022.01.011","url":null,"abstract":"<div><p>Developing high efficient Pd-based electrocatalysts for oxygen reduction reaction (ORR) is still challenging for alkaline membrane fuel cell, since the strong oxygen adsorption energy and easy agglomerative intrinsic properties. In order to simultaneously solve these problems, Pd/Co<sub>3</sub>O<sub>4</sub>–N–C multidimensional materials with porous structures is designed as the ORR catalysts. In details, the ZIF-67 with polyhedral structure was firstly synthesized and then annealed at high-temperature to prepare the N-doped Co<sub>3</sub>O<sub>4</sub> carbon-based material, which was used to homogeneously confine Pd nanoparticles and obtained the Pd/Co<sub>3</sub>O<sub>4</sub>–N–C series catalysts. The formation of Co–N and C–N bond could provide efficient active sites for ORR. Simultaneously, the strong electronic interaction in the interface between the Pd and N-doped Co<sub>3</sub>O<sub>4</sub> could disperse and avoid the agglomeration of Pd nanoparticles and ensure the exposure of active sites, which is crucial to lower the energy barrier toward ORR and substantially enhance the ORR kinetics. Hence, the Pd/Co<sub>3</sub>O<sub>4</sub>–N–C nanocompounds exhibited excellent ORR catalytic performance, ideal Pd mass activity, and durability in 0.1 mol L<sup>−1</sup> KOH solution compared with Co<sub>3</sub>O<sub>4</sub>–N–C and Pd/C. The scalable synthesis method, relatively low cost, and excellent electrochemical ORR performance indicated that the obtained Pd/Co<sub>3</sub>O<sub>4</sub>–N–C electrocatalyst had the potential for application on fuel cells.</p></div>","PeriodicalId":12744,"journal":{"name":"Green Energy & Environment","volume":"8 4","pages":"Pages 1205-1215"},"PeriodicalIF":13.3,"publicationDate":"2023-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"50175398","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}