Carbon-thin-layer protected WP with no passivation supported on acid-treated expanded graphite as efficient Pt Co-catalysts for methanol oxidation and oxygen reduction reactions
Carbon-thin-layer protected WP with no passivation supported on acid-treated expanded graphite as efficient Pt Co-catalysts for methanol oxidation and oxygen reduction reactions
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碳薄层保护的可湿性粉剂，无钝化，负载在酸处理的膨胀石墨上，作为甲醇氧化和氧还原反应的有效 Pt 助催化剂
DOI：
10.1039/c8ta08285e
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发表时间：
2018-11
影响因子：
11.9
通讯作者：
Zou Jinlong
中科院分区：
文献类型：
--
作者：
Zhang Chunyue;Dai Ying;Chen Hun;Ma Yuanyuan;Jing Baojian;Cai Zhuang;Duan Yaqiang;Tang Bo;Zou Jinlong
用于甲醇氧化反应（MOR）/氧还原反应（ORR）的铂基催化剂活性低、稳定性差、CO/甲醇耐受性低，阻碍了直接甲醇燃料电池（DMFC）的应用。在这项研究中，通过一步合成路线合成了磷化钨嵌入碳薄层/酸处理膨胀石墨（WP-CL/AEG）复合材料作为MOR/ORR的Pt载体/助催化剂。对于MOR，Pt-WP-CL/AEG-3（前驱体中P与AEG的摩尔比为3.6）显示出最高的电化学表面积（123.05 m2 gPt−1）和质量活性（2217.6 mA mgPt−1），分别比商业Pt/C（64.16 m2 gPt−1和499.2 mA）高1.92和4.44倍。 mgPt−1)。 Pt-WP-CL/AEG 催化剂还表现出比 Pt/C 更高的 CO 耐受性和稳定性。此外，Pt-WP-CL/AEG-3在酸性介质中也表现出比Pt/C更高的ORR活性，主要通过4e−转移途径（OH−作为主要产物）进行ORR。正如预期的那样，AEG 极大地增强了 Pt-WP-CL/AEG 催化剂的电荷转移能力； WP上W原子诱导暴露的P活性位点促进MOR/ORR过程中甲醇/O2的吸附和活化；来自柠檬酸的CL可以保护WP在空气中不被氧化，从而有助于P活性位点的高活性和稳定性；电荷通过连接的 CL 从 AEG（带正电荷）转移到 WP，然后从 WP 转移到 Pt，这有助于 Pt-WP-CL/AEG 的高 MOR/ORR 活性。这表明 WP-CL/AEG 可以被认为是 MOR/ORR 中 Pt 有前途的载体/助催化剂。
Application of direct methanol fuel cells (DMFCs) is hampered by the low activity, poor stability, and low CO/methanol tolerance of Pt-based catalysts used for methanol oxidation reaction (MOR)/oxygen reduction reaction (ORR). In this study, tungsten phosphide-embedded carbon-thin-layer/acid-treated expanded graphite (WP-CL/AEG) composites are synthesized as Pt-supports/co-catalysts for MOR/ORR via a one-step synthesis route. For MOR, Pt-WP-CL/AEG-3 (molar ratio of P to AEG is 3.6 in precursor) shows the highest electrochemical surface area (123.05 m2 gPt−1) and mass activity (2217.6 mA mgPt−1), which are respectively 1.92 and 4.44 times higher than those of commercial Pt/C (64.16 m2 gPt−1 and 499.2 mA mgPt−1). Pt-WP-CL/AEG catalysts also exhibit higher CO tolerance and stability than Pt/C. Moreover, Pt-WP-CL/AEG-3 also exhibits a higher ORR activity than Pt/C in acidic media, mainly via a 4e− transfer pathway (OH− as the main product) for ORR. As expected, AEG greatly enhances the charge transfer capacity of Pt-WP-CL/AEG catalysts; the exposed P active sites induced by W atoms on WP facilitate methanol/O2 adsorption and activation during MOR/ORR; the CL originated from citric acid can protect WP from being oxidized in air, which contributes to high activity and stability of P active sites; and charges are transferred from AEG (positively charged) to WP via the linked-CL and then from WP to Pt, which contributes to the high MOR/ORR activity of Pt-WP-CL/AEG. It indicates that WP-CL/AEGs can be considered as promising supports/co-catalysts for Pt in MOR/ORR.
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