Exposure of CuSSZ13 to CO 2 at temperatures below 300 8C can deactivate its low-temperature deNOx activity during NH 3 /SCR, with the severity of deactivation being dependent on reaction temperature. The adsorption of NO on Cu 2 + ion is inhibited by CO 2 due to its competitive adsorption, while NH 3 adsorption on acidic sites of CuSSZ13 is largely unaffected by CO 2 , as evidenced by NO-and NH 3 -TPD in the presence of CO 2 . Under O 2 -rich conditions, CO 2 forms unidentate carbonates on Cu 2 + sites suppressing the formation of nitrates, a key reaction intermediate essential for NOx reduction during the NH 3 /SCR reaction, as revealed in an in situ FTIR study.Selective catalytic reduction (SCR) of NO x by urea (urea/SCR) is one of the most efficient and reliable technologies to remove NO x from diesel engine exhaust to meet ever-tightening emission regulations including EURO VI and SULEV without any direct fuel penalty.[1] ZSM5-based catalysts, including CuZSM5 and Mn-Fe/ZSM5, have been regarded as representative urea/ SCR catalysts, mainly owing to their high deNO x activity in the low-temperature region [2] suitable for diesel exhaust temperatures of the advanced engine, for example, the homogenous charge-compression ignition engine, for high fuel efficiency. [3] However, those catalysts still suffer from hydrothermal deactivation during the regeneration of the diesel particulate filter-(>750 8C), which hampers their commercial application to the diesel after-treatment system, [4] although the addition of Er has significantly improved the hydrothermal stability of the Mn-Fe/ ZSM5 catalyst. [2b] In recent years, small-pore zeolite catalysts such as CuSSZ13 and CuSAPO34 have been touted as commercial urea/SCR catalysts owing to their robust hydrothermal stability as well as their excellent low-temperature deNO x activity.[5] Moreover, the CuSSZ13 catalyst has shown high resistance toward hydrocarbon poisoning.[6] Although extensive studies have been conducted to understand the exceptional hydrothermal stability of the CuSSZ13 catalyst, there has been no systematic investigation on the effect of CO 2 on the catalytic activity of CuSSZ13 even though CO 2 is always abundantly present in the exhaust gas stream at approximately 10 %. Indeed, Hudson et al. recently reported that CO 2 molecules are readily adsorbed on the surface of SSZ13.[7] Thus, it is highly desirable and timely to study the effect of CO 2 on the deNO x performance of CuSSZ13 for the urea/SCR, a de facto NH 3 /SCR.We examined the CO 2 -induced deactivation of Cu-(3 wt %)SSZ13 by long-term durability tests in the presence of 10 % CO 2 . To understand the deactivation mechanism of CuSSZ13, the effect of CO 2 on the adsorption of NO x and NH 3 on CuSSZ13 was also investigated by NO x and NH 3 temperature-programmed desorption (TPD) and surface IR spectroscopy studies.The deNO x performance of CuSSZ13 prepared in the present study was examined in the NH 3 /SCR, as depicted in the inset of Figure 1. In the absence of CO 2 , CuSSZ13 revealed excell...