By applying the definition,
$$S_0=\emptyset\\
S_1=\{\text{true},\text{false},0\}\\
S_2=\{\text{true},\text{false},0,\\
\text{succ}(\text{true}) ,
\text{pred}(\text{true}) ,
\text{iszero}(\text{true}) ,\\
\text{succ}(\text{false}) ,
\text{pred}(\text{false}) ,
\text{iszero}(\text{false}) ,\\
\text{succ}(0) ,
\text{pred}(0) ,
\text{iszero}(0) ,\\
\text{if }(\text{true})\text{ then }(\text{true})\text{ else }(\text{true}) ,\\
\text{if }(\text{true})\text{ then }(\text{true})\text{ else }(\text{false}) ,\\
\text{if }(\text{true})\text{ then }(\text{true})\text{ else }(0) ,\\
\text{if }(\text{true})\text{ then }(\text{false})\text{ else }(\text{true}) ,\\
\text{if }(\text{true})\text{ then }(\text{false})\text{ else }(\text{false}) ,\\
\text{if }(\text{true})\text{ then }(\text{false})\text{ else }(0) ,\\
\text{if }(\text{true})\text{ then }(0)\text{ else }(\text{true}) ,\\
\text{if }(\text{true})\text{ then }(0)\text{ else }(\text{false}) ,\\
\text{if }(\text{true})\text{ then }(0)\text{ else }(0) ,\\
\text{if }(\text{false})\text{ then }(\text{true})\text{ else }(\text{true}) ,\\
\text{if }(\text{false})\text{ then }(\text{true})\text{ else }(\text{false}) ,\\
\text{if }(\text{false})\text{ then }(\text{true})\text{ else }(0) ,\\
\text{if }(\text{false})\text{ then }(\text{false})\text{ else }(\text{true}) ,\\
\text{if }(\text{false})\text{ then }(\text{false})\text{ else }(\text{false}) ,\\
\text{if }(\text{false})\text{ then }(\text{false})\text{ else }(0) ,\\
\text{if }(\text{false})\text{ then }(0)\text{ else }(\text{true}) ,\\
\text{if }(\text{false})\text{ then }(0)\text{ else }(\text{false}) ,\\
\text{if }(\text{false})\text{ then }(0)\text{ else }(0) ,\\
\text{if }(0)\text{ then }(\text{true})\text{ else }(\text{true}) ,\\
\text{if }(0)\text{ then }(\text{true})\text{ else }(\text{false}) ,\\
\text{if }(0)\text{ then }(\text{true})\text{ else }(0) ,\\
\text{if }(0)\text{ then }(\text{false})\text{ else }(\text{true}) ,\\
\text{if }(0)\text{ then }(\text{false})\text{ else }(\text{false}) ,\\
\text{if }(0)\text{ then }(\text{false})\text{ else }(0) ,\\
\text{if }(0)\text{ then }(0)\text{ else }(\text{true}) ,\\
\text{if }(0)\text{ then }(0)\text{ else }(\text{false}) ,\\
\text{if }(0)\text{ then }(0)\text{ else }(0)\}
$$
The expansion of $S_3$ is huge ($59475$ terms). That of $S_4$ astronomical ($210379467994775$ terms).