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71.
Liangxu Lin Liang Huang Chang Wu Yu Gao Naihua Miao Chao Wu Aaron T. Marshall Yi Zhao Jiazhao Wang Jun Chen Shixue Dou Gordon G. Wallace Wei Huang 《Angewandte Chemie (International ed. in English)》2023,62(49):e202315182
The exploration of inexpensive and efficient catalysts for oxygen reduction reaction (ORR) is crucial for chemical and energy industries. Carbon materials have been proved promising with different catalysts enabling 2 and 4e− ORR. Nevertheless, their ORR activity and selectivity is still complex and under debate in many cases. Many structures of these active carbon materials are also chemically unstable for practical implementations. Unlike the well-discussed structures, this work presents a strategy to promote efficient and stable 2e− ORR of carbon materials through the synergistic effect of lattice distortion and H-passivation (on the distorted structure). We show how these structures can be formed on carbon cloth, and how the reproducible chemical adsorption can be realized on these structures for efficient and stable H2O2 production. The work here gives not only new understandings on the 2e− ORR catalysis, but also the robust catalyst which can be directly used in industry. 相似文献
72.
Dr. Ningxia Gu Zeyuan Sun Dr. Lixin Song Prof. Dr. Pingfan Du Prof. Dr. Jie Xiong 《Chemphyschem》2023,24(14):e202200919
The perovskite solar cells (PSCs) with high efficiency and stability are in great demand for commercial applications. Although the remarkable photovoltaic feature of perovskite layer plays a great role in improving the PCE of PSCs, the inevitable defects and poor stability of perovskite, etc. are the bottleneck and restrict the commercialization of PSCs. Herein, a review provides a strategy of applying aggregation-induced emission (AIE) molecules, containing passivation functional groups and distinct AIE character, which serves as the alternative materials for fabricating high-efficiency and high-stability PSCs. The methods of introducing AIE molecules to PSCs are also summarized, including additive engineering, interfacial engineering, hole transport materials and so on. In addition, the functions of AIE molecule are discussed, such as defects passivation, morphology modulation, well-matched energy level, enhanced stability, hole transport ability, carrier recombination suppression. Finally, the detailed functions of AIE molecules are offered and further research trend for high performance PSCs based on AIE materials is proposed. 相似文献
73.
Heng Liu Luozhen Jiang Javid Khan Xinxin Wang Jiamin Xiao Handong Zhang Haijiao Xie Prof. Lina Li Prof. Shuangyin Wang Prof. Lei Han 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2023,135(3):e202214988
The regulation of electron distribution of single-atomic metal sites by atomic clusters is an effective strategy to boost their intrinsic activity of oxygen reduction reaction (ORR). Herein we report the construction of single-atomic Mn sites decorated with atomic clusters by an innovative combination of post-adsorption and secondary pyrolysis. The X-ray absorption spectroscopy confirms the formation of Mn sites via Mn-N4 coordination bonding to FeMn atomic clusters (FeMnac/Mn-N4C), which has been demonstrated theoretically to be conducive to the adsorption of molecular O2 and the break of O−O bond during the ORR process. Benefiting from the structural features above, the FeMnac/Mn-N4C catalyst exhibits excellent ORR activity with half-wave potential of 0.79 V in 0.5 M H2SO4 and 0.90 V in 0.1 M KOH as well as preeminent Zn-air battery performance. Such synthetic strategy may open up a route to construct highly active catalysts with tunable atomic structures for diverse applications. 相似文献
74.
Dr. Hong-Tao Zhang Dr. Fei Xie Yu-Hua Guo Yao Xiao Prof. Dr. Ming-Tian Zhang 《Angewandte Chemie (International ed. in English)》2023,62(48):e202310775
We report herein the first nonheme CuFe oxygen reduction catalyst ([CuII(bpbp)(μ-OAc)2FeIII]2+, CuFe−OAc ), which serves as a functional model of cytochrome c oxidase and can catalyze oxygen reduction to water with a turnover frequency of 2.4×103 s−1 and selectivity of 96.0 % in the presence of Et3NH+. This performance significantly outcompetes its homobimetallic analogues (2.7 s−1 of CuCu−OAc with %H2O2 selectivity of 98.9 %, and inactive of FeFe−OAc ) under the same conditions. Structure-activity relationship studies, in combination with density functional theory calculation, show that the CuFe center efficiently mediates O−O bond cleavage via a CuII(μ-η1 : η2-O2)FeIII peroxo intermediate in which the peroxo ligand possesses distinctive coordinating and electronic character. Our work sheds light on the nature of Cu/Fe heterobimetallic cooperation in oxygen reduction catalysis and demonstrates the potential of this synergistic effect in the design of nonheme oxygen reduction catalysts. 相似文献
75.
High-mobility and strong luminescent materials are essential as an important component of organic photodiodes, having received extensive attention in the field of organic optoelectronics. Beyond the conventional chemical synthesis of new molecules, pressure technology, as a flexible and efficient method, can tune the electronic and optical properties reversibly. However, the mechanism in organic materials has not been systematically revealed. Here, we theoretically predicted the pressure-depended luminescence and charge transport properties of high-performance organic optoelectronic semiconductors, 2,6-diphenylanthracene (DPA), by first-principle and multi-scale theoretical calculation methods. The dispersion-corrected density functional theory (DFT-D) and hybrid quantum mechanics/molecular mechanics (QM/MM) method were used to get the electronic structures and vibration properties under pressure. Furthermore, the charge transport and luminescence properties were calculated with the quantum tunneling method and thermal vibration correlation function. We found that the pressure could significantly improve the charge transport performance of the DPA single crystal. When the applied pressure increased to 1.86 GPa, the hole mobility could be doubled. At the same time, due to the weak exciton coupling effect and the rigid flat structure, there is neither fluorescence quenching nor obvious emission enhancement phenomenon. The DPA single crystal possesses a slightly higher fluorescence quantum yield ~ 0.47 under pressure. Our work systematically explored the pressure-dependence photoelectric properties and explained the inside mechanism. Also, we proposed that the external pressure would be an effective way to improve the photoelectric performance of organic semiconductors. 相似文献
76.
《中国化学快报》2021,32(8):2427-2432
Developing high-efficiency,inexpensive,and steady non-precious metal oxygen reduction reaction(ORR) catalysts to displace Pt-based catalysts is significant for commercial applications of Al-air battery.Here,we have prepared the Cu/Cu_2 O-NC catalyst with excellent ORR performance and high stability,due to the synergistic effect of Cu and Cu_2 O nanoparticles.The half-wave potential(0.8 V) and the limiting-current density(5.20 mA/cm~2) of the Cu/Cu_2 O-NC are very close to those of the 20% Pt/C catalyst(0.82 V,5.10 mA/cm~2).Besides,it exhibits excellent performance with a maximal power density of 250 mW/cm~2 and a stable continuous discharge for more than 90 h in the Al-air battery test The promoting effects of Cu_2 O towards Cu-based ORR catalysts are illustrated as follows:(ⅰ) Cu_2 O is the major ORR active site by the redox of Cu(Ⅱ)/Cu(Ⅰ),which provides excellent ORR activities;(ⅱ) Cu can stabilize the location of Cu_2 O by assisting the electron transfer to Cu(Ⅱ)/Cu(Ⅰ) redox,which is conducive to the high stability of the catalyst.This work provides a useful strategy for enhancing the ORR performance of Cu-based catalysts. 相似文献
77.
《中国化学快报》2021,32(9):2597-2616
Electrochemical overall water splitting is attracting a broad focus as a promising strategy for converting the electrical output of renewable resources into chemical fuels, specifically oxygen and hydrogen. However, the urgent challenge in water electrolysis is to search for low-cost, high-efficiency catalysts based on earth-abundant elements as an alternative to the high-cost but effective noble metal-based catalysts. The transition metal-based catalysts are more appealing than the noble metal catalysts because of its low cost, high performance and long stability. Some recent advances for the development in overall water splitting are reviewed in terms of transition metal-based oxides, carbides, phosphides, sulfides, and hybrids of their mixtures as hybrid bifunctional electrocatalysts. Concentrating on different catalytic mechanisms, recent advances in their structural design, controllable synthesis, mechanistic insight, and performance-enhancing strategies are proposed. The challenges and prospects for the future development of transition metal-based bifunctional electrocatalysts are also addressed. 相似文献
78.
《中国化学快报》2021,32(11):3579-3583
Surface oxidized iron-nickel nanorods coupling with reduced graphene architectures (FeNi-O-rGA) are successfully constructed via hydrothermal, freeze-drying, and thermal activation approaches. The hierarchical structure can provide lots of pathways for fast ion diffusion and charge transfer, and expose abundant catalytic sites. Meanwhile, the activity of FeNi-O-rGA is boosted by the optimized metal-oxygen bond strength in FeNi3 alloys. Partial oxidized FeNi nanorods are strongly coupled with rGA by the formation of metal-O-C bonds, which can impede the aggregation of FeNi3 alloys and increase the utilization of active sites. The special structure and partially oxidized FeNi nanorods for FeNi-O-rGA can result in excellent OER activity and catalytic stability. Only 215 mV of overpotential is required to drive the current density of 10 mA/cm2 as well as the Tafel slope of 50.9 mV/dec in 1 mol/L KOH. The change of surface chemistry of FeNi-O-rGA is confirmed by XPS after the OER test, which indicates the highly catalytic stability of FeNi-O-rGA due to the formation of intermediate metal oxyhydroxide. 相似文献
79.
目前,有机-无机杂化钙钛矿太阳能电池(PSC)的器件效率已经超过25%。电子传输层作为PSC中的重要组成部分在提取和传输光生电子,阻挡空穴,修饰界面,调节界面能级和减少电荷复合等方面起着关键作用。无机n型材料,例如TiO2、ZnO、SnO2和其他金属氧化物材料具有成本低和稳定性好的特点,经常在传统PSC中被用作电子传输层(ETL)。有机n型材料,例如富勒烯及其衍生物、萘二酰亚胺聚合物和小分子,具有良好的成膜性能及强的电子传输性能,经常在反式PSC中被用作ETL。本综述详细介绍了PSC中电子传输层的作用机理和制备方法;重点总结了金属氧化物材料、有机分子材料、复合材料和多层分子材料电子传输层和其改性手段的最新研究进展;最后,展望了电子传输层材料朝着高性能PSC的实际应用和发展前景。 相似文献
80.
在河水与海水的交界处实现渗透能提取与捕获是解决未来能源危机的重要方式之一. 渗透能因为储量大, 容易获取以及绿色可持续的优势受到广泛关注. 反向电渗析技术是一种能够有效捕获渗透能的方法之一, 目前已经得到了深入的研究与发展. 离子交换膜是反向电渗析技术转换渗透能的关键组件, 其性能的优异程度决定能量转换效率的高低. 常见的膜材料主要是高分子聚合物及其改性化合物, 最近一些二维材料如石墨烯、 氧化石墨烯、 二硫化钼、 各种框架材料及其改性复合物因优异的选择性离子传输、 纳米级通道、 丰富的表面功能基团以及可修饰性成为捕获渗透能的重要膜材料. 本文综合评述了二维材料作为离子传输通道的类型以及相应的传输机理; 例举了二维材料及其复合物的设计方案和在渗透能转换方面的具体应用; 最后提出了目前二维材料在渗透能转换领域中面临的挑战以及未来的发展方向. 相似文献