氮修饰炭黑负载PdCu合金催化甲酸分解制氢性能研究

Study of catalytic performance of nitrogen modified carbon black supported PdCu alloy for decomposition of formic acid to hydrogen

以氮修饰的炭黑为载体制备负载型PdCu/N-CB系列催化剂,相比较于未经氮修饰的催化剂,其催化性能显著提高,其中Pd8Cu2/N-CB催化剂活性最高,TOF为718.56 h-1,并呈现良好稳定性。通过XRD、TEM、FTIR和XPS等表征分析,结果表明,经APTMS处理所制得的氮修饰载体N-CB促进了所负载的PdCu合金纳米颗粒变得细小并呈现良好的分散性,活性相PdCu合金与氮修饰的载体N-CB之间存在强相互作用,调变合金颗粒表面化学态,提高了催化剂催化甲酸分解制氢性能。通过引入过渡金属和氮修饰载体来改善负载型贵金属催化剂催化性能的方法有助于低成本高性能制氢催化剂开发。

The supported PdCu/N-CB catalysts were prepared by using nitrogen-modified carbon black as support. Compared with the catalysts without nitrogen modification, their catalytic performance in terms of hydrogen production from formic acid was significantly improved. Among them, Pd_(8)Cu_(2)/N-CB catalyst demonstrated the highest activity with TOF of 718.56 h-1 and satisfying stability. XRD, TEM, FTIR and XPS analysis confirm that the N-CB support modified by APTMS can promote the particle size of PdCu alloy to become smaller, which allows better dispersion. The strong interaction between the active phase PdCu alloy and the N-CB support improved the chemical state of PdCu alloy and thereby enhanced the catalytic performance for hydrogen production from formic acid. The method of improving the catalytic performance of supported noble metal catalysts by introducing transition metals and nitrogen modified supports is helpful to the development of low-cost and high-performance hydrogen production catalysts.