Pub Date : 2024-06-29DOI: 10.1016/j.mtener.2024.101640
Jiale He, Weiwei Li, Ruixue Pang, Peng Lu, Meiyun Zhang, Ronghua Feng, Bin Yang
Excellent ionic conductivity and mechanical robustness are significant for separators of Li–S batteries. Aramid nanofiber (ANF) has been widely used in separators due to their excellent mechanical properties and high-temperature resistance. However, pure ANF separator possesses a dense pore structure resulting from the closely intertwined nanofibrous network, leading to inferior ionic conductivity. Herein, we propose a strategy of inhibiting of hydrogen bonding (IHB) among nanofibers to regulate the pore structure of ANF separators via employing pore-forming agent, solvation, and differentiated drying methods. Notably, a graph theoretical methodology (structural GT) is introduced to analyze the percolating network of ANF separator, revealing that the higher average nodal connectivity, the more abundant and homogeneous porous structure and higher conductivity. Excitingly, the pore size and the ionic conductivity of ANF separator by supercritical carbon dioxide drying (S-ANFs) is 44 nm and 0.171 mS/cm, which is 5 times and 1.9 times higher than pure ANF separator, respectively. Moreover, the ANF separator is dimensionally stable under 200 °C, demonstrating its desirable security under extreme conditions. Finally, the half-cell equipped resultant S-ANFs exhibits outstanding cycling stability (566 mAh/g after 200 cycles at 0.5 C) and Coulombic efficiency (99.25%). This work provides an efficient strategy to regulate the pore structure of ANF separator.
{"title":"Regulating pore structure of aramid nanofiber (ANF) separators for lithium–sulfur (Li–S) batteries","authors":"Jiale He, Weiwei Li, Ruixue Pang, Peng Lu, Meiyun Zhang, Ronghua Feng, Bin Yang","doi":"10.1016/j.mtener.2024.101640","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101640","url":null,"abstract":"Excellent ionic conductivity and mechanical robustness are significant for separators of Li–S batteries. Aramid nanofiber (ANF) has been widely used in separators due to their excellent mechanical properties and high-temperature resistance. However, pure ANF separator possesses a dense pore structure resulting from the closely intertwined nanofibrous network, leading to inferior ionic conductivity. Herein, we propose a strategy of inhibiting of hydrogen bonding (IHB) among nanofibers to regulate the pore structure of ANF separators via employing pore-forming agent, solvation, and differentiated drying methods. Notably, a graph theoretical methodology (structural GT) is introduced to analyze the percolating network of ANF separator, revealing that the higher average nodal connectivity, the more abundant and homogeneous porous structure and higher conductivity. Excitingly, the pore size and the ionic conductivity of ANF separator by supercritical carbon dioxide drying (S-ANFs) is 44 nm and 0.171 mS/cm, which is 5 times and 1.9 times higher than pure ANF separator, respectively. Moreover, the ANF separator is dimensionally stable under 200 °C, demonstrating its desirable security under extreme conditions. Finally, the half-cell equipped resultant S-ANFs exhibits outstanding cycling stability (566 mAh/g after 200 cycles at 0.5 C) and Coulombic efficiency (99.25%). This work provides an efficient strategy to regulate the pore structure of ANF separator.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"54 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141781873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Defect-rich transition-metal oxide electrocatalysts hold great promise for alkaline water electrolysis due to their enhanced activity and stability. This study presents a new strategy that significantly improve the OER activity of Co-oxide nanosheets through incorporation of B and P (B/P-CoO NS), eventually leading to abundant surface defects and oxygen vacancies. The B/P-CoO NS demonstrates low overpotential of 220 mV to achieve 10 mA/cm. The electrochemical and kinetic studies coupled with conventional morphological and structural characterizations, reveal that various crystalline defects like vacancies, dislocations, twin planes, and grain boundaries play crucial roles in promoting the OH ion adsorption, the formation of intermediates, and the desorption of oxygen molecules. The industrial viability of the developed electrocatalyst is substantiated through assessments under harsh industrial conditions of 6 M KOH at 60 °C in a zero-gap single-cell alkaline electrolyzer which achieves 1 A/cm at 1.95 V. Chronoamperometry tests (100 h) highlight remarkable robustness of the electrocatalyst. This work establishes a new strategy to fabricate defect-rich OER electrocatalysts, setting a precedent to achieve better OER rates with non-noble materials.
富含缺陷的过渡金属氧化物电催化剂具有更高的活性和稳定性,因此在碱性水电解方面大有可为。本研究提出了一种新策略,通过加入 B 和 P(B/P-CoO NS),最终产生丰富的表面缺陷和氧空位,从而显著提高氧化钴纳米片的 OER 活性。B/P-CoO NS 具有 220 mV 的低过电位,可达到 10 mA/cm。电化学和动力学研究以及传统的形态和结构特征分析表明,空位、位错、孪晶面和晶界等各种晶体缺陷在促进 OH 离子吸附、中间产物形成和氧分子解吸方面起着至关重要的作用。在零间隙单电池碱性电解槽中,在 60 °C、6 M KOH 的苛刻工业条件下进行了评估,在 1.95 V 的电压下达到 1 A/cm 的电流,从而证实了所开发电催化剂的工业可行性。计时器测试(100 小时)凸显了该电催化剂的卓越稳健性。这项工作确立了一种制造富缺陷 OER 电催化剂的新策略,为利用非贵金属材料实现更高的 OER 率开创了先例。
{"title":"Unveiling the kinetics of oxygen evolution reaction in defect-engineered B/P-incorporated cobalt-oxide electrocatalysts","authors":"Aniruddha Bhide, Suraj Gupta, Rinkoo Bhabal, Maulik Patel, Mounib Bahri, Rohan Fernandes, Nainesh Patel","doi":"10.1016/j.mtener.2024.101638","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101638","url":null,"abstract":"Defect-rich transition-metal oxide electrocatalysts hold great promise for alkaline water electrolysis due to their enhanced activity and stability. This study presents a new strategy that significantly improve the OER activity of Co-oxide nanosheets through incorporation of B and P (B/P-CoO NS), eventually leading to abundant surface defects and oxygen vacancies. The B/P-CoO NS demonstrates low overpotential of 220 mV to achieve 10 mA/cm. The electrochemical and kinetic studies coupled with conventional morphological and structural characterizations, reveal that various crystalline defects like vacancies, dislocations, twin planes, and grain boundaries play crucial roles in promoting the OH ion adsorption, the formation of intermediates, and the desorption of oxygen molecules. The industrial viability of the developed electrocatalyst is substantiated through assessments under harsh industrial conditions of 6 M KOH at 60 °C in a zero-gap single-cell alkaline electrolyzer which achieves 1 A/cm at 1.95 V. Chronoamperometry tests (100 h) highlight remarkable robustness of the electrocatalyst. This work establishes a new strategy to fabricate defect-rich OER electrocatalysts, setting a precedent to achieve better OER rates with non-noble materials.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"59 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613137","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Titanium niobium oxides are promising anode materials for sodium-ion batteries (SIBs) due to their efficient ion diffusion channels. However, their poor electronic conductivity impedes the longevity of SIBs. To address these issues, core@shell TiNbO/C@C microspheres (TNO/C@C) have been developed to enhance electron conduction. The TNO/C@C, featuring a bulk and surface dual conductive configuration, outperforms pure TNO and other control samples such as TNO/C and TNO@C that rely solely on either bulk or surface electronic conductors. Thus, the TNO/C@C achieves a fast-charging rate of 200 C, allowing full charging in 2 s, and demonstrates long-term stability over 10,000 cycles. Raman analysis reveals a zero-strain feature during sodiation/desodiation, which minimizes structural degradation over repeated cycles. electrochemical impedance spectroscopy test indicates low electron resistance, enhancing both the rate capability and stability. Therefore, the bulk and surface dual conducting strategy offers new insights into robust and fast-charging SIBs.
{"title":"Pseudocapacitive TiNb0.8O4 microspheres for fast-charging and durable sodium storage","authors":"Xinyuan Li, Tianyi Zhang, Zhuo Chen, Hao Fan, Ping Hu, Congcong Cai, Liang Zhou","doi":"10.1016/j.mtener.2024.101637","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101637","url":null,"abstract":"Titanium niobium oxides are promising anode materials for sodium-ion batteries (SIBs) due to their efficient ion diffusion channels. However, their poor electronic conductivity impedes the longevity of SIBs. To address these issues, core@shell TiNbO/C@C microspheres (TNO/C@C) have been developed to enhance electron conduction. The TNO/C@C, featuring a bulk and surface dual conductive configuration, outperforms pure TNO and other control samples such as TNO/C and TNO@C that rely solely on either bulk or surface electronic conductors. Thus, the TNO/C@C achieves a fast-charging rate of 200 C, allowing full charging in 2 s, and demonstrates long-term stability over 10,000 cycles. Raman analysis reveals a zero-strain feature during sodiation/desodiation, which minimizes structural degradation over repeated cycles. electrochemical impedance spectroscopy test indicates low electron resistance, enhancing both the rate capability and stability. Therefore, the bulk and surface dual conducting strategy offers new insights into robust and fast-charging SIBs.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"41 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613138","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-25DOI: 10.1016/j.mtener.2024.101636
Yusuf Khan, Vinayak S. Kale, Jehad K. El-Demellawi, Yongjiu Lei, Wenli Zhao, Sharath Kandambeth, Prakash T. Parvatkar, Osama Shekhah, Mohamed Eddaoudi, Husam N. Alshareef
The growing demand for emerging electronic applications, including energy storage, sensors, and portable devices, has created a pressing need to develop miniaturized flexible energy storage components with convenient device architecture. Here, we report an in-plane hybrid micro-supercapacitor made of covalent organic frameworks and TiCT MXene as positive and negative electrodes, respectively. The devices utilize three-dimensional laser-scribed graphene (LSG) as a current collector for both electrodes using a CO-laser-based technique due to its good resolution for in-plane device fabrication, and high porosity of LSG that can facilitate better rate performance. The constructed hybrid supercapacitor has a maximum areal capacitance of 131.46 mF/cm and a voltage window of 1.2 V. The findings provide a new strategy to fabricate a hybrid supercapacitor for self-powered device applications at the microscale.
{"title":"Hybrid microsupercapacitors based on Ti3C2Tx MXene and covalent organic frameworks","authors":"Yusuf Khan, Vinayak S. Kale, Jehad K. El-Demellawi, Yongjiu Lei, Wenli Zhao, Sharath Kandambeth, Prakash T. Parvatkar, Osama Shekhah, Mohamed Eddaoudi, Husam N. Alshareef","doi":"10.1016/j.mtener.2024.101636","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101636","url":null,"abstract":"The growing demand for emerging electronic applications, including energy storage, sensors, and portable devices, has created a pressing need to develop miniaturized flexible energy storage components with convenient device architecture. Here, we report an in-plane hybrid micro-supercapacitor made of covalent organic frameworks and TiCT MXene as positive and negative electrodes, respectively. The devices utilize three-dimensional laser-scribed graphene (LSG) as a current collector for both electrodes using a CO-laser-based technique due to its good resolution for in-plane device fabrication, and high porosity of LSG that can facilitate better rate performance. The constructed hybrid supercapacitor has a maximum areal capacitance of 131.46 mF/cm and a voltage window of 1.2 V. The findings provide a new strategy to fabricate a hybrid supercapacitor for self-powered device applications at the microscale.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"137 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141781753","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-24DOI: 10.1016/j.mtener.2024.101633
Muhammad Yousaf, Yuzheng Lu, Muhammad Akbar, Lei Lei, Shao Jing, Youkun Tao
Solid oxide fuel cells (SOFCs) are promising for clean energy generation due to their high efficiency, fuel flexibility, and status as a clean energy source with no environmental hazards. However, the challenge of operating these SOFCs at elevated temperatures (800–1000 °C) presents significant hurdles regarding material selection, cost-effectiveness, and device fabrication. Lowering the operational temperature of SOFCs can enhance performance and economic viability. Nevertheless, this pursuit introduces challenges in the form of increased ohmic and polarization resistances, which detrimentally affect electrochemical performance. High ohmic resistance and activation energy at lower temperatures reduce ionic conductivity and impede SOFC device efficiency. Recent advancements in materials and cutting-edge technologies have addressed these issues, particularly in low-temperature operations for SOFC devices. This review article focuses on the latest developments in material selection and advanced technologies that have demonstrated notable improvements in power output and long-term durability at lower operating temperatures, highlighting the significance of high-performing electrolyte and electrode materials with enhanced electrochemical and fast electrocatalytic functionality to improve cell efficiency. Additionally, the article explores the significant obstacles encountered by SOFCs at low operating temperatures.
{"title":"Advances in solid oxide fuel cell technologies: lowering the operating temperatures through material innovations","authors":"Muhammad Yousaf, Yuzheng Lu, Muhammad Akbar, Lei Lei, Shao Jing, Youkun Tao","doi":"10.1016/j.mtener.2024.101633","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101633","url":null,"abstract":"Solid oxide fuel cells (SOFCs) are promising for clean energy generation due to their high efficiency, fuel flexibility, and status as a clean energy source with no environmental hazards. However, the challenge of operating these SOFCs at elevated temperatures (800–1000 °C) presents significant hurdles regarding material selection, cost-effectiveness, and device fabrication. Lowering the operational temperature of SOFCs can enhance performance and economic viability. Nevertheless, this pursuit introduces challenges in the form of increased ohmic and polarization resistances, which detrimentally affect electrochemical performance. High ohmic resistance and activation energy at lower temperatures reduce ionic conductivity and impede SOFC device efficiency. Recent advancements in materials and cutting-edge technologies have addressed these issues, particularly in low-temperature operations for SOFC devices. This review article focuses on the latest developments in material selection and advanced technologies that have demonstrated notable improvements in power output and long-term durability at lower operating temperatures, highlighting the significance of high-performing electrolyte and electrode materials with enhanced electrochemical and fast electrocatalytic functionality to improve cell efficiency. Additionally, the article explores the significant obstacles encountered by SOFCs at low operating temperatures.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"2 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141781874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-24DOI: 10.1016/j.mtener.2024.101635
Peng-Jun Deng, Yaxuan Wang, Yang Liu, Jiajia Lu, Han-Pu Liang
Developing electrolytic seawater catalysts with excellent performance is crucial for efficient hydrogen production. In this study, NiP nanoparticles anchored on NiMo oxides, denoted as NiMo-P, are synthesized through heat-induced aliquation and phosphating of Ni in the ammonium nickel molybdate. Physicochemical characterizations reveal that the abundant NiP nanoparticles are uniformly distributed on NiMo oxides. Electrochemical data reveal that a mere overpotential of 103 mV is sufficient to achieve −100 mA cm in alkaline simulated seawater, which is significantly lower than that of Pt foil (179 mV) and commercial Pt/C (165 mV). This remarkable activity observed in NiMo-P may be due to the superior water dissociation activity and hydrogen desorption ability of the NiP nanoparticles, as calculated by density functional theory, which surpasses that of Pt. Meanwhile, the NiMo-P exhibits outstanding stability, as evidenced by the chronoamperometric curve. The current remains at 98.1% of its initial value after 500 h, which can be attributed to the etching-hydrolysis method that strengthens the catalyst-carrier interaction. Besides, the inherent repulsion toward chlorine ions at the cathode effectively avoids chemical corrosion. Importantly, when coupled with the previously reported anode, NiMo-P also exhibits exceptional performance in alkaline seawater.
{"title":"Heat-induced aliquation and phosphating of nickel as efficient catalysts for hydrogen evolution in alkaline seawater","authors":"Peng-Jun Deng, Yaxuan Wang, Yang Liu, Jiajia Lu, Han-Pu Liang","doi":"10.1016/j.mtener.2024.101635","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101635","url":null,"abstract":"Developing electrolytic seawater catalysts with excellent performance is crucial for efficient hydrogen production. In this study, NiP nanoparticles anchored on NiMo oxides, denoted as NiMo-P, are synthesized through heat-induced aliquation and phosphating of Ni in the ammonium nickel molybdate. Physicochemical characterizations reveal that the abundant NiP nanoparticles are uniformly distributed on NiMo oxides. Electrochemical data reveal that a mere overpotential of 103 mV is sufficient to achieve −100 mA cm in alkaline simulated seawater, which is significantly lower than that of Pt foil (179 mV) and commercial Pt/C (165 mV). This remarkable activity observed in NiMo-P may be due to the superior water dissociation activity and hydrogen desorption ability of the NiP nanoparticles, as calculated by density functional theory, which surpasses that of Pt. Meanwhile, the NiMo-P exhibits outstanding stability, as evidenced by the chronoamperometric curve. The current remains at 98.1% of its initial value after 500 h, which can be attributed to the etching-hydrolysis method that strengthens the catalyst-carrier interaction. Besides, the inherent repulsion toward chlorine ions at the cathode effectively avoids chemical corrosion. Importantly, when coupled with the previously reported anode, NiMo-P also exhibits exceptional performance in alkaline seawater.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"40 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613139","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-24DOI: 10.1016/j.mtener.2024.101629
S. Pandiaraj, S. Aftab, G. Koyyada, F. Kabir, H.H. Hegazy, J.H. Kim
In recent years, perovskite photovoltaics (PVs) have emerged as a highly promising technology for solar energy conversion. However, challenges such as instability, hysteresis, and limited device lifetimes have impeded their commercialization. In light of this, the proposed review addresses these critical issues by exploring the application of two-dimensional (2D) and one-dimensional (1D) carbon-based materials as interfacial layers in perovskite solar cells (PSCs). A potential remedy for these problems is the use of interfacial layers between the charge transport and perovskite absorber layers. In recent times, there has been a lot of interest in carbon-based materials in both two- and one-dimensional forms as interfacial materials because of their special qualities and suitability for PSCs. The application of 2D or 1D materials as interfacial layers in perovskite PVs is reviewed in this review, including electron (or hole) transport layers (ETLs or HTLs). We list the main issues with PSCs and show how these issues can be lessened by using interfacial layers. Furthermore, we synthesize existing understanding of the potential of 2D materials and their contribution in resolving important PSC problems. This thorough analysis advances the creation of dependable and effective perovskite PV systems for real-world solar energy harvesting uses.
{"title":"Perovskite photovoltaics: exploring the role of 2D and 1D carbon-based interfacial layers for enhanced stability and efficiency","authors":"S. Pandiaraj, S. Aftab, G. Koyyada, F. Kabir, H.H. Hegazy, J.H. Kim","doi":"10.1016/j.mtener.2024.101629","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101629","url":null,"abstract":"In recent years, perovskite photovoltaics (PVs) have emerged as a highly promising technology for solar energy conversion. However, challenges such as instability, hysteresis, and limited device lifetimes have impeded their commercialization. In light of this, the proposed review addresses these critical issues by exploring the application of two-dimensional (2D) and one-dimensional (1D) carbon-based materials as interfacial layers in perovskite solar cells (PSCs). A potential remedy for these problems is the use of interfacial layers between the charge transport and perovskite absorber layers. In recent times, there has been a lot of interest in carbon-based materials in both two- and one-dimensional forms as interfacial materials because of their special qualities and suitability for PSCs. The application of 2D or 1D materials as interfacial layers in perovskite PVs is reviewed in this review, including electron (or hole) transport layers (ETLs or HTLs). We list the main issues with PSCs and show how these issues can be lessened by using interfacial layers. Furthermore, we synthesize existing understanding of the potential of 2D materials and their contribution in resolving important PSC problems. This thorough analysis advances the creation of dependable and effective perovskite PV systems for real-world solar energy harvesting uses.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"8 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613141","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-06-24DOI: 10.1016/j.mtener.2024.101634
Shuyu Bu, Bin Liu, Anquan Zhu, Chuhao Luan, Kai Liu, Qili Gao, Xin Kong, Guo Hong, Wenjun Zhang
The development of high-efficiency catalysts plays a crucial role in advancing CO electroreduction techniques. Among potential candidates, diamond-based electrocatalysts show promise due to their broad electrochemical windows, which effectively suppress competitive hydrogen evolution and ensure high CO reduction efficiency. In this study, we report an integrated electrode composed of oxygen-terminated diamond nanocone (OD) with CoPc-molecules anchoring (CoPc/OD). The CoPc/OD electrodes exhibited remarkable performance, achieving a maximum Faradaic efficiency (FE) of 94.1% for CO at −0.97 V vs reversible hydrogen electrode (RHE), and maintaining an FE higher than 80% over a wide potential range of −0.67 V to −1.07 V vs RHE. The outstanding performance of the CoPc/OD electrode can be attributed to the synergistic effects between the nanostructured diamond surface and the CoPc catalyst. The hydroxyl-rich nature of the diamond surface facilitates the anchoring of CoPc molecules and bonding with Co atoms in CoPc. Simultaneously, the nanostructured diamond with sharp tips enhances CO adsorption, thereby improving the catalyst's performance. This study provides valuable insights into the utilization of non-metallic carbon materials, particularly diamond, as metal-free catalysts in CO electrochemical reduction and tackles challenges such as low current density and poor Faradaic efficiency, thus contributing to the advancement of more effective catalysts for CO electroreduction.
高效催化剂的开发在推进一氧化碳电还原技术方面发挥着至关重要的作用。在潜在的候选催化剂中,基于金刚石的电催化剂因其宽广的电化学窗口而大有可为,它能有效抑制竞争性氢进化并确保较高的 CO 还原效率。在本研究中,我们报告了一种由氧端金刚石纳米锥(OD)和 CoPc 分子锚定(CoPc/OD)组成的集成电极。CoPc/OD 电极表现出卓越的性能,在 -0.97 V 与可逆氢电极 (RHE) 相比时,对 CO 的最大法拉第效率 (FE) 达到 94.1%,并且在 -0.67 V 至 -1.07 V 与 RHE 相比的宽电位范围内,FE 保持在 80% 以上。CoPc/OD 电极的出色性能可归因于纳米结构金刚石表面与 CoPc 催化剂之间的协同效应。金刚石表面富含羟基的性质有利于 CoPc 分子的锚定以及与 CoPc 中 Co 原子的结合。同时,具有尖锐尖端的纳米结构金刚石增强了对 CO 的吸附,从而提高了催化剂的性能。这项研究为利用非金属碳材料(尤其是金刚石)作为一氧化碳电化学还原中的无金属催化剂提供了宝贵的见解,并解决了低电流密度和低法拉第效率等难题,从而有助于开发更有效的一氧化碳电还原催化剂。
{"title":"Oxygen functionalized diamond nanocone arrays coupling cobalt phthalocyanine for enhanced electrochemical CO2 reduction","authors":"Shuyu Bu, Bin Liu, Anquan Zhu, Chuhao Luan, Kai Liu, Qili Gao, Xin Kong, Guo Hong, Wenjun Zhang","doi":"10.1016/j.mtener.2024.101634","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101634","url":null,"abstract":"The development of high-efficiency catalysts plays a crucial role in advancing CO electroreduction techniques. Among potential candidates, diamond-based electrocatalysts show promise due to their broad electrochemical windows, which effectively suppress competitive hydrogen evolution and ensure high CO reduction efficiency. In this study, we report an integrated electrode composed of oxygen-terminated diamond nanocone (OD) with CoPc-molecules anchoring (CoPc/OD). The CoPc/OD electrodes exhibited remarkable performance, achieving a maximum Faradaic efficiency (FE) of 94.1% for CO at −0.97 V vs reversible hydrogen electrode (RHE), and maintaining an FE higher than 80% over a wide potential range of −0.67 V to −1.07 V vs RHE. The outstanding performance of the CoPc/OD electrode can be attributed to the synergistic effects between the nanostructured diamond surface and the CoPc catalyst. The hydroxyl-rich nature of the diamond surface facilitates the anchoring of CoPc molecules and bonding with Co atoms in CoPc. Simultaneously, the nanostructured diamond with sharp tips enhances CO adsorption, thereby improving the catalyst's performance. This study provides valuable insights into the utilization of non-metallic carbon materials, particularly diamond, as metal-free catalysts in CO electrochemical reduction and tackles challenges such as low current density and poor Faradaic efficiency, thus contributing to the advancement of more effective catalysts for CO electroreduction.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"25 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613140","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
This study focuses on the kinetic analysis of chlorophyll-based dimer photosensitizers adsorbed on Pt/TiO photocatalyst for light-driven hydrogen evolution. To elucidate the detailed mechanism, four photosensitizers, a carboxylated chlorin () and its dimer derivatives connecting an accessory pigment of chlorin (), porphyrin (), and bacteriochlorin () were synthesized and their kinetic processes in photocatalytic hydrogen evolution were investigated. The results indicate that possesses the highest ability to produce photogenerated carriers, with an appropriate excited state lifetime, lowest propensity for charge recombination, and longest charge transfer lifetime. These favorable characteristics contribute to its exceptional photocatalytic activity compared with other photosensitizers. Specifically, the -sensitized Pt/TiO photocatalyst exhibits a remarkable hydrogen generation rate of 5.36 mmol/g/h. Moreover, these photosensitizers demonstrate excellent stability and multiple-experimental consistency. This study provides significant insights into the development of dyad photosensitizers and highlights their practical significance in the field of photocatalysis. By harnessing chlorophyll, we have successfully harnessed efficient and controlled hydrogen fuel generation through photocatalytic water splitting, thus paving the way for future advancements in clean and sustainable energy production.
{"title":"Kinetic analysis of TiO2-based photocatalysts sensitized with chlorophyll-derived dimers for light-driven hydrogen evolution","authors":"Tianfang Zheng, Aijun Li, Hongyu Tu, Lingyun Pan, Shin-ichi Sasaki, Xiao-Feng Wang","doi":"10.1016/j.mtener.2024.101631","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101631","url":null,"abstract":"This study focuses on the kinetic analysis of chlorophyll-based dimer photosensitizers adsorbed on Pt/TiO photocatalyst for light-driven hydrogen evolution. To elucidate the detailed mechanism, four photosensitizers, a carboxylated chlorin () and its dimer derivatives connecting an accessory pigment of chlorin (), porphyrin (), and bacteriochlorin () were synthesized and their kinetic processes in photocatalytic hydrogen evolution were investigated. The results indicate that possesses the highest ability to produce photogenerated carriers, with an appropriate excited state lifetime, lowest propensity for charge recombination, and longest charge transfer lifetime. These favorable characteristics contribute to its exceptional photocatalytic activity compared with other photosensitizers. Specifically, the -sensitized Pt/TiO photocatalyst exhibits a remarkable hydrogen generation rate of 5.36 mmol/g/h. Moreover, these photosensitizers demonstrate excellent stability and multiple-experimental consistency. This study provides significant insights into the development of dyad photosensitizers and highlights their practical significance in the field of photocatalysis. By harnessing chlorophyll, we have successfully harnessed efficient and controlled hydrogen fuel generation through photocatalytic water splitting, thus paving the way for future advancements in clean and sustainable energy production.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"38 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141548826","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Because of their good chemical stability and excellent optical properties, MoO, WO, and BiWO are important in photochromism. Their light-to-color conversion is highly dependent on the electronic band structure and charge transfer, and they obey the mechanism of electron accumulation in semiconductors when excited within the bandgap. Pure semiconductors face limitations in practical applications due to insufficient light absorption, charge carrier recombination, and low charge capacity. Diverse forms of photochromic hybrids (nanopowders, films, hydrogels, and multilayer structures) with rapid change, repeatability, and reversibility are possible via nanocustomization, surface/interface engineering, heterojunction fabrication, and complexing organic ligands. Manipulating the function of photochromic systems through light stimulation is becoming an attractive paradigm, divided into two branches: light-color complementarity and photoconductivity. This review examines the widely accepted photoresponsive principles and the still controversial energy transfer models. We emphasize the correlation between material properties and performance enhancement to inspire the rational structure design. The bottlenecks in current development are identified by analyzing application-specific innovation concepts, fabrication processes, and performance metrics. In addition, we present several perspectives to encourage meaningful multidisciplinary collaboration.
{"title":"Light-to-color conversion on MoO3, WO3, and Bi2WO6: from mechanism to materials and applications","authors":"Xu Dong, Yongjuan Dang, Zhengyu Wu, Yindong Tong, Xianhua Liu, Yiren Lu","doi":"10.1016/j.mtener.2024.101632","DOIUrl":"https://doi.org/10.1016/j.mtener.2024.101632","url":null,"abstract":"Because of their good chemical stability and excellent optical properties, MoO, WO, and BiWO are important in photochromism. Their light-to-color conversion is highly dependent on the electronic band structure and charge transfer, and they obey the mechanism of electron accumulation in semiconductors when excited within the bandgap. Pure semiconductors face limitations in practical applications due to insufficient light absorption, charge carrier recombination, and low charge capacity. Diverse forms of photochromic hybrids (nanopowders, films, hydrogels, and multilayer structures) with rapid change, repeatability, and reversibility are possible via nanocustomization, surface/interface engineering, heterojunction fabrication, and complexing organic ligands. Manipulating the function of photochromic systems through light stimulation is becoming an attractive paradigm, divided into two branches: light-color complementarity and photoconductivity. This review examines the widely accepted photoresponsive principles and the still controversial energy transfer models. We emphasize the correlation between material properties and performance enhancement to inspire the rational structure design. The bottlenecks in current development are identified by analyzing application-specific innovation concepts, fabrication processes, and performance metrics. In addition, we present several perspectives to encourage meaningful multidisciplinary collaboration.","PeriodicalId":18277,"journal":{"name":"Materials Today Energy","volume":"60 1","pages":""},"PeriodicalIF":9.3,"publicationDate":"2024-06-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141613142","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}