To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabiliz...To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic activity.Herein,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable OER.It is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination sites.These sites function to anchor and stabilize single Ir single atoms on the support.The strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn catalyst.With a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2) and a small Tafel slope of 35 mV·dec^(−1) for the OER in a 1 M KOH solution.These results significantly surpass the performance of the commercially available IrO_(2) catalyst.展开更多
Bimetallic nanocrystals (BMNCs) with distinguished electronic and chemical properties from those of their parent metals,offer the opportunity to obtain new catalysts with enhanced selectivity,activity,and stability.He...Bimetallic nanocrystals (BMNCs) with distinguished electronic and chemical properties from those of their parent metals,offer the opportunity to obtain new catalysts with enhanced selectivity,activity,and stability.Here we describe the facile synthesis of rhodium-copper bimetallic system with different compositions and uniform morphology for chemo selective hydrogenation of functionalized quinolines.Our findings demonstrate that Rh-Cu BMNCs exhibited composition dependent activity and selectivity.BMNCs with rhodium to copper ratio 3:1 surpassed individual Rh and Cu and other compositions both in activity and selectivity for quinolines hydrogenation and performed even better than Rh/C with same amount of Rh.Rh3Cui catalyst displayed excellent tolerance for synthetically significant functional groups such as -OH,NH2,F,particularly for aldehyde group which is very reactive towards reduction.These results suggested that the coexistence of rhodium and copper metals play important role in the enhancement of catalytic activity due to synergistic effects and revealed that bimetallic nanocrystals can be promising as practical catalysts for selective hydrogenation of quinoline and other substrates.展开更多
基金supported by the National Key R&D Program of China(No.2021YFF0500500)National Natural Science Foundation of China(Nos.21925202 and U22B2071)+1 种基金Yunnan Provincial Science and Technology Project at Southwest United Graduate School(No.202302AO370017)International Joint Mission on Climate Change and Carbon Neutrality.
文摘To address the sluggish kinetics of the oxygen evolution reaction(OER),a potential approach is to rationally design and fabricate extremely effective single atom catalysts(SACs).Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic activity.Herein,we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide(Ir-SAC/NiFeZn-LDH)electrocatalyst for highly efficient and stable OER.It is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination sites.These sites function to anchor and stabilize single Ir single atoms on the support.The strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn catalyst.With a loading Ir content of 1.09 wt.%,this catalyst demonstrates a highly stable OER activity,with an overpotential of 196 mV at 10 mA·cm^(−2) and a small Tafel slope of 35 mV·dec^(−1) for the OER in a 1 M KOH solution.These results significantly surpass the performance of the commercially available IrO_(2) catalyst.
基金supported by the National Key R&D Program of China (Nos.2016YFA0202801 and 2017YFA0700101)the National Natural Science Foundation of China (Nos.21573119,21590792,21890383,and 21872076)China Postdoctoral Science Foundation (No.2018M631444).
文摘Bimetallic nanocrystals (BMNCs) with distinguished electronic and chemical properties from those of their parent metals,offer the opportunity to obtain new catalysts with enhanced selectivity,activity,and stability.Here we describe the facile synthesis of rhodium-copper bimetallic system with different compositions and uniform morphology for chemo selective hydrogenation of functionalized quinolines.Our findings demonstrate that Rh-Cu BMNCs exhibited composition dependent activity and selectivity.BMNCs with rhodium to copper ratio 3:1 surpassed individual Rh and Cu and other compositions both in activity and selectivity for quinolines hydrogenation and performed even better than Rh/C with same amount of Rh.Rh3Cui catalyst displayed excellent tolerance for synthetically significant functional groups such as -OH,NH2,F,particularly for aldehyde group which is very reactive towards reduction.These results suggested that the coexistence of rhodium and copper metals play important role in the enhancement of catalytic activity due to synergistic effects and revealed that bimetallic nanocrystals can be promising as practical catalysts for selective hydrogenation of quinoline and other substrates.