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一石二鸟:解锁非晶态氢氧化镍与钯纳米晶体在乙醇和甲酸氧化反应中的协同作用

One Stone Two Birds: Unlocking the Synergy between Amorphous Ni(OH) and Pd Nanocrystals toward Ethanol and Formic Acid Oxidation.

作者信息

Yang Hu, Zhang Aichuang, Bai Yunfei, Chu Mingyu, Li Han, Liu Yuan, Zhu Peng, Chen Xiaolei, Deng Chengwei, Yuan Xiaolei

机构信息

School of Chemistry and Chemical Engineering, Nantong University, 9 Seyuan Road, Nantong 226019, China.

Space Power Technology State Key Laboratory, Shanghai Institute of Space Power-Sources, 2965 Dongchuan Road, Shanghai 200245, China.

出版信息

Inorg Chem. 2022 Sep 12;61(36):14419-14427. doi: 10.1021/acs.inorgchem.2c02307. Epub 2022 Aug 29.

Abstract

Even though extensive efforts have been devoted to mixing Pd nanocrystals with Ni(OH) for the enhanced synergy, it remains a great challenge to incorporate nanosized Ni(OH) species on the Pd electrode and reveal their synergy. Herein, we present spongelike Pd nanocrystals with the modification of amorphous Ni(OH) species. The catalyst configuration is first considered by compositing Pd with Ni(OH) species to optimize the Pd-Pd interatomic distance and then constructing a strongly coupled interface between Pd nanostructures and Ni(OH) species. For the ethanol oxidation reaction (EOR) and the formic acid oxidation reaction (FAOR), Pd-Ni(OH) composites exhibit an impressive mass activity of 4.98 and 2.65 A mg, respectively. Most impressively, there is no significant decrease in the EOR activity during five consecutive cycles (50 000 s). A series of CO-poisoning tests have proved that the enhanced EOR and FAOR performances involve synergy between Pd nanostructures and Ni(OH) species.

摘要

尽管人们为了增强协同效应,在将钯纳米晶体与氢氧化镍混合方面付出了巨大努力,但在钯电极上引入纳米尺寸的氢氧化镍物种并揭示它们的协同效应仍然是一个巨大的挑战。在此,我们展示了具有非晶态氢氧化镍物种修饰的海绵状钯纳米晶体。首先通过将钯与氢氧化镍物种复合来考虑催化剂构型,以优化钯-钯原子间距离,然后在钯纳米结构和氢氧化镍物种之间构建强耦合界面。对于乙醇氧化反应(EOR)和甲酸氧化反应(FAOR),钯-氢氧化镍复合材料分别表现出令人印象深刻的4.98和2.65 A mg的质量活性。最令人印象深刻的是,在连续五个循环(50 000 s)中,EOR活性没有显著下降。一系列的一氧化碳中毒测试证明,增强的EOR和FAOR性能涉及钯纳米结构和氢氧化镍物种之间的协同作用。

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