Interfacial Proton-Relay Microenvironment Enables Self-Driven Singlet Oxygen Generation under Neutral Conditions

Area of Science:

• Catalysis
• Green Chemistry
• Environmental Science

Background:

• Activating molecular oxygen (O2) to singlet oxygen (1O2) under neutral conditions is crucial for green oxidation chemistry.
• Existing methods are limited by slow proton-coupled OOH formation and desorption.

Purpose of the Study:

• To engineer an interfacial proton-relay microenvironment for energy-free O2 to 1O2 conversion.
• To enable self-driven O2 activation without external energy inputs for oxidation chemistry.

Main Methods:

• Designed a catalyst with MoS2 and CuCl to create an interfacial proton-relay microenvironment.
• Utilized electron-deficient sulfur sites in MoS2 as a proton reservoir.
• Facilitated proton migration through Cu-S-Mo channels to activate O2 on Cu sites.

Main Results:

• Achieved self-driven O2 to 1O2 conversion without external energy.
• Demonstrated accelerated OOH hydrogenation and suppressed O-O bond cleavage.
• Attained quantitative pollutant removal with sustained operation (>16 h) in pilot-scale membrane filtration.

Conclusions:

• The interfacial proton-relay design overcomes proton-transfer limitations in O2 activation.
• This approach offers a general strategy for sustainable oxidation and environmental remediation using transition metal sulfides.
• The engineered system advances autonomous catalytic platforms for green chemistry.