PDF(Pubmed)
Abstract：
The development of alternative clean energy carriers is a key challenge for our society. Carbon-based hydrogen storage materials are well-suited to undergo reversible (de)hydrogenation reactions and the development of catalysts for the individual process steps is crucial. In the current state, noble metal-based catalysts still dominate this field. Here, a system for partially reversible and carbon-neutral hydrogen storage and release is reported. It is based on the dual-functional roles of formamides and uses a small molecule Fe-pincer complex as the catalyst, showing good stability and reusability with high productivity. Starting from formamides, quantitative production of CO-free hydrogen is achieved at high selectivity ( > 99.9%). This system works at modest temperatures of 90 °C, which can be easily supplied by the waste heat from e.g., proton-exchange membrane fuel cells. Employing such system, we achieve >70% H2 evolution efficiency and >99% H2 selectivity in 10 charge-discharge cycles, avoiding undesired carbon emission between cycles.
摘要：
替代清洁能源载体的发展是我们社会面临的关键挑战。碳基储氢材料非常适合进行可逆(去)氢化反应,并且开发用于各个工艺步骤的催化剂是至关重要的。在当前状态下,基于贵金属的催化剂仍然主导该领域。这里,报告了一种部分可逆和碳中性的储氢和释放系统。它基于甲酰胺的双重功能作用，并使用小分子Fe-钳形络合物作为催化剂，表现出良好的稳定性和可重用性，生产率高。从甲酰胺开始，在高选择性(>99.9%)下实现了无CO氢的定量生产。该系统在90°C的适度温度下工作，这可以很容易地由来自例如，质子交换膜燃料电池。采用这样的系统，我们在10个充放电循环中实现>70%的H2析出效率和>99%的H2选择性，避免循环之间不希望的碳排放。
