温和条件下金属氧化物中的阳离子交换(CE)仍然是定制其组成并实现实际应用的必要但具有挑战性的目标。在这里,我们首先开发了一种非晶化诱导策略,以实现室温CE,用于普遍合成单原子掺杂的In2O3纳米片(NSs)。密度泛函理论(DFT)计算表明,a-In2O3NS中存在的大量配位不饱和位点有助于克服CE反应的能垒。根据经验,作为主体材料的a-In2O3NS成功地与一元阳离子(Cu2+,Co2+,Mn2+,Ni2+),二元阳离子(Co2+Mn2+,Co2+Ni2+,Mn2+Ni2+),和三元阳离子(Co2+Mn2+Ni2+)。令人印象深刻的是,获得了高负载的单原子掺杂(超过10原子%)In2O3NS。此外,Cu/a-In2O3NS具有出色的乙醇产率(798.7μmolg-1h-1),对CO2光还原的选择性高达99.5%。这项工作提供了一种在温和条件下在金属氧化物中诱导CE反应的新方法,并为关键应用构建了可扩展的单原子掺杂催化剂。
Cation exchange (CE) in metal oxides under mild conditions remains an imperative yet challenging goal to tailor their composition and enable practical applications. Herein, we first develop an amorphization-induced strategy to achieve room-temperature CE for universally synthesizing single-atom doped In2O3 nanosheets (NSs). Density functional theory (DFT) calculations elucidate that the abundant coordination-unsaturated sites present in a-In2O3 NSs are instrumental in surmounting the energy barriers of CE reactions. Empirically, a-In2O3 NSs as the host materials successfully undergo exchange with unary cations (Cu2+, Co2+, Mn2+, Ni2+), binary cations (Co2+Mn2+, Co2+Ni2+, Mn2+Ni2+), and ternary cations (Co2+Mn2+Ni2+). Impressively, high-loading single-atom doped (over 10 atom %) In2O3 NSs were obtained. Additionally, Cu/a-In2O3 NSs exhibit an excellent ethanol yield (798.7 μmol g-1 h-1) with a high selectivity of 99.5% for the CO2 photoreduction. This work offers a new approach to induce CE reactions in metal oxides under mild conditions and constructs scalable single-atom doped catalysts for critical applications.