Key Laboratory of Functional Inorganic Material Chemistry, (Ministry of Education of China), School of Chemistry and Materials Science, Heilongjiang University, Harbin, 150080, P. R. China.
ChemSusChem. 2021 Dec 17;14(24):5508-5516. doi: 10.1002/cssc.202101913. Epub 2021 Nov 5.
Although the activity of electrocatalysts towards oxygen evolution reaction (OER) has achieved considerable improvement by modulating the intrinsic electron structure, the role of supports to OER performance, often being reduced to enhancing the conductivity, is not fully explored. In this paper, a proof-of-concept study based on a series of hybrids of nickel iron (hydr)oxide nanoparticles (NiFeO NPs) and carbon supports with different oxidation level compared the motivation of supports for OER activity. The key to implementation lay in anchoring and growing of NiFeO NPs on the various carbon supports by electrostatic assembly and subsequent in-situ reduction. A series of experiments indicated that the strong coupling of metal ions and graphene oxide (GO) contributed to the formation of ultrasmall NiFeO NPs (≈2 nm) and the firm interaction between NiFeO NPs and GO, which in turn resulted in exposing more metal atoms, modulating local electron structure of active sites, and accelerating the charge-transfer ability. The OER activity of optimal NiFeO NPs anchored on rGO (NiFeO NPs/rGO) was significantly elevated, achieving an overpotential as small as 201 mV at 10 mA cm and a low Tafel slope of 68 mV dec , as well as remarkable stability. Such exciting capacity for catalyzing OER prevailed over the vast majority of previously reported transition-metal electrocatalysts, even superior to numerous noble metal-containing catalysts. The electrolyzer employing NiFeO NPs/rGO and commercial Pt/C for anode and cathode could be powered by a solar cell for efficient alkaline seawater splitting. This work opens up a universal and scalable way for further advancing the intrinsic activity of energy-related materials.
尽管通过调节内在电子结构,电催化剂在氧气析出反应(OER)中的活性已经得到了相当大的提高,但支撑物对 OER 性能的作用,通常被简化为增强导电性,并没有得到充分的探索。在本文中,我们进行了一项基于一系列镍铁(氢)氧化物纳米颗粒(NiFeO NPs)与具有不同氧化水平的碳载体的杂化体的概念验证研究,比较了支撑物对 OER 活性的影响。实现这一目标的关键在于通过静电组装和随后的原位还原将 NiFeO NPs 锚定并生长在各种碳载体上。一系列实验表明,金属离子与氧化石墨烯(GO)的强耦合有助于形成超小的 NiFeO NPs(≈2nm),并增强了 NiFeO NPs 与 GO 之间的牢固相互作用,进而导致更多金属原子的暴露、活性位点局部电子结构的调节以及电荷转移能力的加速。最佳 NiFeO NPs 锚定在还原氧化石墨烯(rGO)上的(NiFeO NPs/rGO)的 OER 活性显著提高,在 10 mA cm 时的过电势仅为 201 mV,塔菲尔斜率低至 68 mV dec ,并且具有出色的稳定性。这种对 OER 催化的令人兴奋的能力超过了之前报道的绝大多数过渡金属电催化剂,甚至优于许多含贵金属的催化剂。采用 NiFeO NPs/rGO 和商业 Pt/C 作为阳极和阴极的电解槽可以由太阳能电池供电,从而实现高效的碱性海水分解。这项工作为进一步提高与能源相关的材料的内在活性开辟了一条通用且可扩展的途径。