The probability of no 4 with four 6-sided dice$(p_1)=(\frac{5}{6})^4$
The probability of exactly one 4 with four 6-sided dice$(p_2)$
$=4\frac{1}{6}(\frac{5}{6})^3$ as here the combinations are $4XXX$ or $X4XX$ or $XX4X$ or $XXX4$ where $X$ is some other face$≠4$
So, the probability of at least two 4s with four 6-sided dice$=1-p_1-p_2$
$=1-((\frac{5}{6})^4+4\frac{1}{6}(\frac{5}{6})^3)$
$=1-(\frac{5}{6})^3(\frac{5}{6}+\frac{4}{6})=1-\frac{125}{144}=\frac{19}{144}$
The probability of throwing at least 4 by one 6-sided dice
$=\frac{3}{6}=\frac{1}{2}$
The possible combinations are $XXYY$, $XYXY$, $XYYX$, $YXXY$, $YXYX$, $YYXX$
where $1≤Y≤3,4≤X≤6$
So, the required probability of throwing exactly two occurrences of at least 4 is $^4C_2\frac{1}{2}\frac{1}{2}(1-\frac{1}{2})(1-\frac{1}{2})=\frac{3}{8}$ using Binomial Distribution.