Concentrating photo-thermo-organized single-atom and 2D-raft Cu catalyst for full-spectrum solar harmonic conversion of aqueous urea and urine into hydrogen

Solar-driven hydrogen evolution from urea-rich wastewater is a highly promising energy-environment bi-functional synthetical solution, while the intrinsic contradict between spectral energy quantity and quality of sunlight limits the existing wavelength-dependent technologies. Herein, we report the first demonstration of concentrated photo-thermo-catalysis (CPTC) technology that regulates the spectral energy quantity and quality and creates the synergy between photon and thermal effects to achieve full-spectrum solar harmonic conversion of aqueous urea and urine into hydrogen. The 50% enhanced CPTC performance compared with sole photo-/thermo-catalysis is achieved due to: (1) Catalyst structure optimization. Single Cu atom and 2D Cu raft are acquired on defect-rich TiO₂ support by photo-thermo-organized metal-support interaction; (2) Reaction pathway expansion. The breakthrough against thermodynamic barrier of urea to hydrogen is realized by the novel cascade reactions of thermally-triggered urea hydrolysis and thermally-assisted ammonia photo-decomposition. The technological viability is convincingly presented through outdoor test with artificial urine under real sunlight.