Updating Intrinsic Activity of Single Atom Site with P-O Bond for Rechargeable Zn-Air Battery.
Updating Intrinsic Activity of Single Atom Site with P-O Bond for Rechargeable Zn-Air Battery.
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DOI：
10.1021/acsami.9b11337
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发表时间：
2019-08
影响因子：
9.5
通讯作者：
He Sun;Sisi Liu;Mengfan Wang;Tao Qian;J. Xiong;Chenglin Yan
中科院分区：
文献类型：
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作者：
He Sun;Sisi Liu;Mengfan Wang;Tao Qian;J. Xiong;Chenglin Yan
锌-空气二次电池在过去的十年里引起了人们的极大关注，但其进一步发展将需要高效的双功能电催化剂来驱动缓慢的阴极反应。虽然单原子催化剂具有最大的金属原子利用率，但其催化性能还远不能令人满意。在这里，我们通过引入P-O键来更新单个原子位点的固有活性，从而降低锌空气电池的反应过电位来解决这个挑战。通过密度泛函理论模拟，证实了P-O键在单原子金属位产生良好的表面电子环境，提高其催化活性中的关键作用。P-O掺杂的原子分散催化剂的实验结果表明，提供优异的双功能性能，具有显着的半波电位为0.89 V的可逆氢电极的氧还原反应和可逆氧电极指数为0.74 V，超过大多数报道的非贵金属催化剂。在实际应用中，水溶液和全固态锌空气电池都表现出上级功率密度和稳定的循环性能，证实了其在下一代电子设备中的潜在可行性。
Rechargeable Zn-air battery has drawn great attention over the last decade but its further development will require efficient bifunctional electrocatalysts to drive the sluggish cathodic reactions. Although single atom catalyst with maximum utilization per metal atom shows great promise, its catalytic performance is still far from satisfaction. Here we tackle this challenge by introducing P-O bond to update the intrinsic activity of single atom site and thus reduce the reaction overpotential of Zn-air battery. The critical role of P-O bond in producing favorable surface electronic environment of the single atom metal site and improving its catalytic activity is identified with density functional theory simulations. The P-O-doped atomically dispersed catalyst is shown experimentally to deliver excellent bifunctional performance, with a remarkable half-wave potential of 0.89 V versus reversible hydrogen electrode for oxygen reduction reaction and a reversible oxygen electrode index of 0.74 V, exceeding most reported nonprecious metal catalysts. When subjected to practical application, both aqueous and all-solid-state Zn-air battery illustrate superior power density and robust cyclic performance, confirming its potential feasibility in next generation electronic devices.