Controllable Increase of Boron Content in B-Pd Interstitial Nanoalloy To Boost the Oxygen Reduction Activity of Palladium
Controllable Increase of Boron Content in B-Pd Interstitial Nanoalloy To Boost the Oxygen Reduction Activity of Palladium
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可控增加B-Pd间隙纳米合金中的硼含量以提高钯的氧还原活性
DOI：
10.1021/acs.chemmater.7b03732
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发表时间：
2017-12-12
影响因子：
8.6
通讯作者：
Chen, Shengli
中科院分区：
文献类型：
--
作者：
Li, Jun;Chen, Junxiang;Chen, Shengli
硼掺杂可以提高钯的催化活性。掺杂含量的精确控制是至关重要的，但在目前的合成中仍然很困难，这通常涉及使用不稳定和昂贵的硼烷有机化合物。本文利用N，N-二甲基甲酰胺（DMF）对Na+较强的溶剂化作用和BH 4-在DMF中稳定性的提高，以NaBH 4为还原剂和硼源，在DMF中合成了B-Pd间隙纳米晶。硼含量可以通过改变反应时间和NaBH 4浓度容易地调节，可以达到高达20原子%。这样的高硼掺杂导致对Pd朝向氧还原反应（ORR）的催化能力的极大有益效果。合成的B-Pd纳米合金表现出ORR的质量和比活性，分别约为。比现有技术的商业Pt催化剂在碱性溶液中的那些高14和14.6倍。密度泛函理论（DFT）计算
Boron doping can boost the catalytic activity of palladium for diverse reactions. Precise control of the doping content is crucial but remains difficult in current synthesis, which generally involves the use of instable and costly borane-organic compounds. Herein, by taking advantage of the relatively strong solvation of N,N-dimethylformamide (DMF) to Na+ and the increased stability BH4– in DMF, we synthesize B-Pd interstitial nanocrystals in DMF, with NaBH4 acting as a reductant and boron source. The boron content, which can be readily tuned by changing the reaction time and NaBH4 concentration, can reach up to 20 at. %. Such a high boron doping results in a great beneficial effect on the catalytic capability of Pd toward the oxygen reduction reaction (ORR). The synthesized B-Pd nanoalloy exhibits a mass and specific activity for ORR that are, respectively, ca. 14 and 14.6 times higher than those of the state-of-the-art commercial Pt catalyst in alkaline solution. Density functional theory (DFT) calculat...