Self-limiting growth of ligand-free ultrasmall bimetallic nanoparticles on carbon through under temperature reduction for highly efficient methanol electrooxidation and selective hydrogenation
Self-limiting growth of ligand-free ultrasmall bimetallic nanoparticles on carbon through under temperature reduction for highly efficient methanol electrooxidation and selective hydrogenation
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DOI：
10.1016/j.apcatb.2019.118553
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发表时间：
2020-05
影响因子：
22.1
通讯作者：
Mingzhen Hu;Lei Jin;Yuanyuan Zhu;Lei Zhang;Xingxu Lu;Peter Kerns;Xingsong Su;Sen Cao;P. Gao-P
中科院分区：
文献类型：
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作者：
Mingzhen Hu;Lei Jin;Yuanyuan Zhu;Lei Zhang;Xingxu Lu;Peter Kerns;Xingsong Su;Sen Cao;P. Gao-P
本文报道了一种低温还原（UTR）法制备碳负载的超小含钯双金属纳米催化剂的自限生长方法。在Pd的存在下，第二贱金属前驱体（M = co， Ni和Zn）的（co）还原温度低于其热力学还原温度时，观察到UTR现象。UTR现象的根源在于Pd的氢外溢在低于其热力学还原温度的温度下驱动母材（co）的还原；同时，进一步的还原被同时停止，以限制纳米颗粒在形成纳米合金时的过度生长。以氮化碳为载体，利用UTR技术，研究了Pd1.7Co、Pd1.6Ni和Pd2Zn三种含pd纳米合金的自限生长，其平均尺寸约为1.5 nm。亚2 nm含pd的双金属纳米合金在肉桂醛的甲醇电氧化和选择性加氢反应中均表现出优异的催化性能。
We report a self-limiting growth method of ultrasmall Pd-containing bimetallic nanocatalysts supported on carbon through under temperature reduction (UTR). The UTR phenomenon is observed for the (co)reduction of a second base metal precursor (M = Co, Ni, and Zn) below its thermodynamic reduction temperature in the presence of Pd. The origin of the UTR phenomenon lies in the hydrogen spillover of Pd to drive the (co)reduction of the base metal at the temperature below its thermodynamic reduction temperature; while, the further reduction is shut down simultaneously to limit the overgrowth of nanoparticles when forming nanoalloys. Using nitrided carbon as a support, we demonstrate the self-limiting growth of three Pd-containing nanoalloys, including Pd1.7Co, Pd1.6Ni and Pd2Zn, with average sizes around 1.5 nm using UTR. Sub-2 nm Pd-containing bimetallic nanoalloys exhibited excellent catalytic properties in both methanol electrooxidation and selective hydrogenation of cinnamaldehyde.