Jinxin Wang, Wei Guo, Mingming Sun, Geng Zhang, Yang Meng and Qiuyu Zhang
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引用次数: 0
Abstract
Aqueous pseudocapacitive storage has shown promise for future energy applications, but it suffers from a single reaction pathway and mechanism that restrain performance breakthroughs, especially under commercial high-mass-loading conditions. Herein, using MnO2 as a pseudocapacitive storage material, we tailored a reversible pseudocapacitive-type electrode/electrolyte interphase (PEI) by refining the cationic environment, which broke the limitation of MnO2 to unlock an energetic dual-ion storage mechanism. Theoretical calculations demonstrated that the engineered dynamic PEI elevated the removal energy of active Mn species to stabilize dual-cation storage and, more importantly, provided highly available MnO2/PEI heterointerface spaces to accommodate more charges. We unveiled that the exceptional heterointerface region with considerable charge redistribution enabled a significantly reduced ion-migration energy barrier compared with that of the pure MnO2 interlayer, contributing to fast “multi-processing” storage of dual carriers. As a proof-of-concept, the tailored mechanism enabled robust stability with 92% capacitance retention after 25 000 cycles. Besides, an appealing areal capacitance of 11.1 F cm−2 was demonstrated under a high mass loading of 27.4 mg cm−2. Our findings signify a paradigm shift in aqueous pseudocapacitive chemistry and offer insights into dynamic microenvironment regulation for building advanced energy storage devices.
在未来的能源技术中,水相赝电容存储显示出前景,但其反应途径和机制单一,限制了性能的突破,特别是在商业高质量负载条件下。在此,我们以MnO2为例,通过改善阳离子环境,定制了一种可逆的伪电容型电极/电解质界面(PEI),首次打破了MnO2的限制,解锁了一个高能双离子存储机制。理论计算表明,设计的动态PEI提高了活性Mn的去除能,以稳定双阳离子的储存,更重要的是,提供了高可用的MnO2/PEI异质界面空间,以容纳更多的电荷。我们发现,与纯二氧化锰中间层相比,具有大量电荷再分配的特殊异质界面区域能够显著降低离子迁移能垒,有助于双载流子的快速“多处理”存储。作为概念验证,定制的机制在25000次循环后具有92%的电容保持率,具有强大的稳定性。此外,在27.4 mg cm-2的高质量载荷下,可以显示出11.1 F cm-2的吸引人的面电容。我们的研究结果表明了水相赝电容化学的范式转变,并为构建先进的储能设备提供了动态微环境调节的见解。
期刊介绍:
Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences."
Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).