Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawba...Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawbacks of low efficiency,poor stability,and low selectivity.Here,a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO_(2)particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO_(2)-to-fuel conversion.An ultrahigh light-to-fuel efficiency up to 35.7%,high production rates of H_(2)(136.6 mmol min^(-1)g^(-1))and CO(148.2 mmol min^(-1)g^(-1)),excellent selectivity(H_(2)/CO ratio of 0.92),and good stability are reported simultaneously.These outstanding performances are attributed to strong metal-support interactions,improved CO_(2)absorption and activation,and decreased apparent activation energy under direct light illumination.MgAlO_(x)@SiO_(2)support helps to lower the activation energy of CH^(*) oxidation to CHO^(*) and improve the dissociation of CH_(4)to CH_(3)^(*) as confirmed by DFT calculations.Moreover,the lattice oxygen of MgAlO_(x) participates in the reaction and contributes to the removal of carbon deposition.This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency,high selectivity,and benign sustainability.展开更多
基金This work was financially supported by the Basic Science Center Program for Ordered Energy Conversion of the National Natural Science Foundation of China(51888103)the National Key R&D Program of China(2021YFF0500700)Jiangsu Natural Science Foundation Project(BE2022024 and BK20202008).
文摘Solar-driven CO_(2)-to-fuel conversion assisted by another major greenhouse gas CH_(4)is promising to concurrently tackle energy shortage and global warming problems.However,current techniques still suffer from drawbacks of low efficiency,poor stability,and low selectivity.Here,a novel nanocomposite composed of interconnected Ni/MgAlOx nanoflakes grown on SiO_(2)particles with excellent spatial confinement of active sites is proposed for direct solar-driven CO_(2)-to-fuel conversion.An ultrahigh light-to-fuel efficiency up to 35.7%,high production rates of H_(2)(136.6 mmol min^(-1)g^(-1))and CO(148.2 mmol min^(-1)g^(-1)),excellent selectivity(H_(2)/CO ratio of 0.92),and good stability are reported simultaneously.These outstanding performances are attributed to strong metal-support interactions,improved CO_(2)absorption and activation,and decreased apparent activation energy under direct light illumination.MgAlO_(x)@SiO_(2)support helps to lower the activation energy of CH^(*) oxidation to CHO^(*) and improve the dissociation of CH_(4)to CH_(3)^(*) as confirmed by DFT calculations.Moreover,the lattice oxygen of MgAlO_(x) participates in the reaction and contributes to the removal of carbon deposition.This work provides promising routes for the conversion of greenhouse gasses into industrially valuable syngas with high efficiency,high selectivity,and benign sustainability.
