Carbon dots regulate the interface electron transfer and catalytic kinetics of Pt-based alloys catalyst for highly efficient hydrogen oxidation

The regulation of interface electron-transfer and catalytic kinetics is very important to design the efficient electrocatalyst for alkaline hydrogen oxidation reaction(HOR).Here,we show the Pt-Ni alloy nanoparticles(PtNi_(2))have an enhanced HOR activity compared with single component Pt catalyst.While,the interface electron-transfer kinetics of PtNi_(2)catalyst exhibits a very wide electron-transfer speed distribution.When combined with carbon dots(CDs),the interface charge transfer of PtNi_(2)-CDs composite is optimized,and then the PtNi_(2)-5 mg CDs exhibits about 2.67 times and 4.04 times higher mass and specific activity in 0.1 M KOH than that of 20%commercial Pt/C.In this system,CDs also contribute to trapping H^(+)and H_(2)O generated during HOR,tuning hydrogen binding energy(HBE),and regulating interface electron transfer.This work provides a deep understanding of the interface catalytic kinetics of Pt-based alloys towards highly efficient HOR catalysts design.

In-situ transient photovoltage study on interface electron transfer regulation of carbon dots/NiCo_(2)O_(4) photocatalyst for the enhanced overall water splitting activity

Photocatalytic hydrogen production by overall water solar-splitting is a prospective strategy to solve energy crisis.However,the rapid recombination of photogenerated electron–hole pairs deeply restricts photocatalytic activity of catalysts.Here,the in-situ transient photovoltage(TPV)technique was developed to investigate the interfacial photogenerated carrier extraction,photogenerated carrier recombination and the interfacial electron delivery kinetics of the photocatalyst.The carbon dots/NiCo_(2)O_(4)(CDs/NiCo_(2)O_(4))composite shows weakened recombination rate of photogenerated carriers due to charge storage of CDs,which enhances the photocatalytic water decomposition activity without any scavenger.CDs can accelerate the interface electron extraction about 0.09 ms,while the maximum electron storage time by CDs is up to 0.7 ms.The optimal CDs/NiCo_(2)O_(4)composite(5 wt.%CDs)displays the hydrogen production of 62µmol·h^(−1)·g^(−1) and oxygen production of 29µmol·h^(−1)·g^(−1) at normal atmosphere,which is about 4 times greater than that of pristine NiCo_(2)O_(4).This work provides sufficient evidence on the charge storage of CDs and the interfacial charge kinetics of photocatalysts on the basis of in-situ TPV tests.

Carbon dots/Bi_(2)WO_(6) composite with compensatory photo-electronic effect for overall water photo-splitting at normal pressure

Overall water photo-splitting is a prospective ideal pathway to produce ultra-clean H_(2) energy by semiconductors.However,the band structure of many semiconductors cannot satisfy the requirement of H_(2) and O_(2) production at the same time.Herein,we illustrate that carbon dots(CDs)/Bi_(2)WO_(6) photocatalyst with compensatory photo-electronic effect has enhanced activity for overall water photo-splitting without any sacrificial agent.In this complex photocatalytic system,the photo-potential provided by CDs makes the CDs/Bi2WO6(C-BWO)composite could satisfy the band structure conditions for overall water photo-splitting.The C-BWO composite(3 wt%CDs content)exhibits optimized hydrogen evolution(oxygen evolution)of 0.28μmol/h(0.12μmol/h)with an approximate 2:1(H_(2):O_(2))stoichiometry at normal pressure.We further employed the in-situ transient photovoltage(TPV)technique to study the photoelectron extraction and the interface charge transfer kinetics of this composite catalyst.