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Self‐Established Rapid Magnesiation/De‐Magnesiation Pathways in Binary Selenium–Copper Mixtures with Significantly Enhanced Mg‐Ion Storage Reversibility
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2017-11-14 , DOI: 10.1002/adfm.201701718 Zhonghua Zhang 1, 2 , Bingbing Chen 1 , Huimin Xu 3 , Zili Cui 1 , Shanmu Dong 1 , Aobing Du 1, 2 , Jun Ma 1 , Qingfu Wang 1 , Xinhong Zhou 3 , Guanglei Cui 1
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2017-11-14 , DOI: 10.1002/adfm.201701718 Zhonghua Zhang 1, 2 , Bingbing Chen 1 , Huimin Xu 3 , Zili Cui 1 , Shanmu Dong 1 , Aobing Du 1, 2 , Jun Ma 1 , Qingfu Wang 1 , Xinhong Zhou 3 , Guanglei Cui 1
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Rechargeable magnesium/sulfur (Mg/S) and magnesium/selenium (Mg/Se) batteries are characterized by high energy density, inherent safety, and economical effectiveness, and therefore, are of great scientific and technological interest. However, elusive challenges, including the limited charge storage capacity, low Coulombic efficiency, and short cycle life, have been encountered due to the sluggish electrochemical kinetics and severe shuttles of ploysulfides (polyselenide). Taking selenium as model paradigm, a new and reliable Mg‐Se chemistry is proposed through designing binary selenium‐copper (Se‐Cu) cathodes. An intriguing effect of Cu powders on the electrochemical reaction pathways of the active Se microparticles is revealed in a way of forming Cu3Se2 intermediates, which induces an unconventional yet reversible two‐stage magnesiation mechanism: Mg‐ions first insert into Cu3Se2 phases; in a second step Cu‐ions in the Mg2xCu3Se2 lattice exchange with Mg‐ions. As expected, binary Se‐Cu electrodes show significantly improved reversibility and elongated cycle life. More bracingly, Se/C nanostructures fabricated by facile blade coating Se nanorodes onto copper foils exhibit high output power and capacity (696.0 mAh g−1 at 67.9 mA g−1), which outperforms all previously reported Mg/Se batteries. This work envisions a facile and reliable strategy to achieve better reversibility and long‐term durability of selenium (sulfur) electrodes.
中文翻译：
在二元硒-铜混合物中自行建立的快速镁化/去镁化途径，具有增强的镁离子可逆性
可再充电的镁/硫（Mg / S）和镁/硒（Mg / Se）电池具有高能量密度，固有安全性和经济效益的特点，因此具有重大的科学技术意义。然而，由于缓慢的电化学动力学和多硫化物（聚硒化物）的剧烈穿梭，已经遇到了难以捉摸的挑战，包括有限的电荷存储容量，低库仑效率和短循环寿命。以硒为模型范式，通过设计二元硒-铜（Se-Cu）阴极，提出了一种新的，可靠的Mg-Se化学方法。以形成Cu 3 Se 2的方式揭示了Cu粉对活性Se微粒的电化学反应路径的吸引作用。中间体，它引起了一种非常规但可逆的两级放大作用机理：Mg离子首先插入Cu 3 Se 2相中；Mg离子首先插入Cu 3 Se 2相中。在第二步中，Mg 2 x Cu 3 Se 2中的Cu离子与Mg离子交换。正如预期的那样，二元Se-Cu电极显示出显着改善的可逆性和延长的循环寿命。更bracingly，硒/ C纳米结构制造由容易刮涂硒nanorodes到铜箔表现出高输出功率和容量（毫安696.0克-1在67.9毫安克-1），其性能优于以前报道的所有Mg / Se电池。这项工作设想了一种简便而可靠的策略，以实现硒（硫）电极更好的可逆性和长期耐用性。
更新日期：2017-11-14
中文翻译：
在二元硒-铜混合物中自行建立的快速镁化/去镁化途径，具有增强的镁离子可逆性
可再充电的镁/硫（Mg / S）和镁/硒（Mg / Se）电池具有高能量密度，固有安全性和经济效益的特点，因此具有重大的科学技术意义。然而，由于缓慢的电化学动力学和多硫化物（聚硒化物）的剧烈穿梭，已经遇到了难以捉摸的挑战，包括有限的电荷存储容量，低库仑效率和短循环寿命。以硒为模型范式，通过设计二元硒-铜（Se-Cu）阴极，提出了一种新的，可靠的Mg-Se化学方法。以形成Cu 3 Se 2的方式揭示了Cu粉对活性Se微粒的电化学反应路径的吸引作用。中间体，它引起了一种非常规但可逆的两级放大作用机理：Mg离子首先插入Cu 3 Se 2相中；Mg离子首先插入Cu 3 Se 2相中。在第二步中，Mg 2 x Cu 3 Se 2中的Cu离子与Mg离子交换。正如预期的那样，二元Se-Cu电极显示出显着改善的可逆性和延长的循环寿命。更bracingly，硒/ C纳米结构制造由容易刮涂硒nanorodes到铜箔表现出高输出功率和容量（毫安696.0克-1在67.9毫安克-1），其性能优于以前报道的所有Mg / Se电池。这项工作设想了一种简便而可靠的策略，以实现硒（硫）电极更好的可逆性和长期耐用性。
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