T he Earth's environment is seriously threatened by an increase in atmospheric carbon dioxide (CO 2 ) concentrations. To support sustainable development in the 21st century, controlling the global warming caused by the increasing atmospheric CO 2 levels has become a main scientific and technological challenge. 1 To prevent catastrophic events related to atmospheric CO 2 , the emission of CO 2 should be reduced as soon as possible. One of the most promising solutions to overcome this challenge is the conversion of CO 2 into valuable chemicals, thus contributing to the reduction of the atmospheric CO 2 load. This process is regarded as one of the most ideal solutions for the "greenhouse effect" problem. Potential techniques have been studied extensively, including FischerÀTropsch reactions, photochemical or electrochemical conversions, catalytic hydrogenation, and producing valuable compounds, such as methanol and methane. 2À5 In recent decades, hydrothermal reactions have received more attention for the treatment of organic wastes and biomass conversion because of the unique inherent properties of hightemperature water (HTW) that include a high ion product (K w ) and a low dielectric constant, which are favorable for promoting reactions without catalysts. 6À9 In our previous studies, it was found that hydrogen can be generated during the hydrothermal cracking of bitumen and polymer wastes, such as polyethylene (PE) and sulfur-containing rubber. 10À14 A cheap source of hydrogen has become the primary challenge in the conversion of CO 2 . Hydrogen is currently produced by reforming hydrocarbons, which is an energy-intensive process. If the hydrogen produced during the hydrothermal cracking of polymer wastes could be directly used to reduce CO 2 , then an efficient process for CO 2 conversion and polymer waste use would be realized.In this study, we examined the possibility of CO 2 reduction during the hydrothermal cracking of polymer wastes. PE, as a representative of plastic waste, and ethylene propylene diene monomer (EPDM), as a model for sulfur-containing waste rubber, were used as test materials. The molecular structure of EPDM can be found in the Supporting Information. Experiments were conducted at temperatures varying from 300 to 450°C in a bomb-type batch reactor with a Hastelloy C-276 inner wall and an inner volume of 42 mL. The reactor was equipped with a highpressure valve to allow for pressure measurements, CO 2 input, and gas sampling. The experimental setup has been described in detail elsewhere. 15 After reactions, gas and liquid samples were collected and analyzed by gas chromatographyÀthermal conductivity detector (GCÀTCD) and gas chromatographyÀmass spectroscopy (GCÀMS), respectively. A more detailed description of experimental procedures and the gas collection method can be found in the Supporting Information.First, experiments with PE were conducted with various temperatures (300À450°C), reaction times, and initial pH values with or without CO 2 . No significant differences were observed in th...