FexNi9-xS8 (x = 3-6) as potential photocatalysts for solar-driven hydrogen production?
FexNi9-xS8 (x = 3-6) as potential photocatalysts for solar-driven hydrogen production?
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DOI：
10.1039/c8fd00173a
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发表时间：
2019-07
影响因子：
3.4
通讯作者：
David Tetzlaff;C. Simon;D. S. Achilleos;M. Smialkowski;Kai junge Puring;A. Bloesser;Stefan M. Piontek;Hatice Kasap;D. Siegmund;E. Reisner;R. Marschall;Ulf‐Peter Apfel
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作者：
David Tetzlaff;C. Simon;D. S. Achilleos;M. Smialkowski;Kai junge Puring;A. Bloesser;Stefan M. Piontek;Hatice Kasap;D. Siegmund;E. Reisner;R. Marschall;Ulf‐Peter Apfel
在温和条件下用非贵金属有效还原质子是我们现代社会面临的挑战。自然界利用氢化酶，包括含铁和含镍活性位点的酶机制，来进行质子到氢的转化。我们在此报告了一种直接的合成途径，该途径指向生物启发材料FexNi 9-xS 8的定义明确的颗粒，FexNi 9-xS 8是氢化酶金属硫簇的结构和功能类似物。此外，pentlandites作为太阳能驱动的H2-生产的光催化剂的潜力进行了评估的第一次。FexNi 9-xS 8材料是可见光响应的（带隙在2.02和2.49 eV之间，取决于镍黄铁矿的Fe：Ni含量），并且显示出接近质子还原的热力学势的导带能量。尽管有限的驱动力，已经观察到光催化H2的适度活性。我们的观察表明，pentlandites作为光催化剂的未来发展的潜力。这项工作为探索仿生化学和材料设计之间的强大协同作用提供了基础，以解锁太阳能转换的新应用。
The efficient reduction of protons by non-noble metals under mild conditions is a challenge for our modern society. Nature utilises hydrogenases, enzymatic machineries that comprise iron- and nickel- containing active sites, to perform the conversion of protons to hydrogen. We herein report a straightforward synthetic pathway towards well-defined particles of the bio-inspired material FexNi9-xS8, a structural and functional analogue of hydrogenase metal sulfur clusters. Moreover, the potential of pentlandites to serve as photocatalysts for solar-driven H2-production is assessed for the first time. The FexNi9-xS8 materials are visible light responsive (band gaps between 2.02 and 2.49 eV, depending on the pentlandite's Fe : Ni content) and display a conduction band energy close to the thermodynamic potential for proton reduction. Despite the limited driving force, a modest activity for photocatalytic H2 has been observed. Our observations show the potential for the future development of pentlandites as photocatalysts. This work provides a basis to explore powerful synergies between biomimetic chemistry and material design to unlock novel applications in solar energy conversion.