You have already two columns: $v_1=\begin{pmatrix}\frac{1}{\sqrt{6}}\\\frac{1}{\sqrt{6}}\\\frac{2}{\sqrt{6}}\end{pmatrix}$ and $v_2=\begin{pmatrix}-\frac{1}{\sqrt{2}}\\\frac{1}{\sqrt{2}}\\0\end{pmatrix}$. Add a new column just to make $(v_1,v_2,u)$ linearly independent. You have a lot of freedom there, choose whatever is the easiest for the subsequent calculation. For example, set $u=\begin{pmatrix}1\\0\\0\end{pmatrix}$.
Now:
- Calculate the new vector:
$$\overline{v_3}=u-\langle u,v_1\rangle v_1-\langle u,v_2\rangle v_2=\begin{pmatrix}1\\0\\0\end{pmatrix}-\frac{1}{\sqrt{6}}\begin{pmatrix}\frac{1}{\sqrt{6}}\\\frac{1}{\sqrt{6}}\\\frac{2}{\sqrt{6}}\end{pmatrix}+\frac{1}{\sqrt{2}}\begin{pmatrix}-\frac{1}{\sqrt{2}}\\\frac{1}{\sqrt{2}}\\0\end{pmatrix}=\begin{pmatrix}\frac{1}{3}\\\frac{1}{3}\\-\frac{1}{3}\end{pmatrix}$$
- Calculate $\|\overline{v_3}\|=\sqrt{\langle \overline{v_3},\overline{v_3}\rangle}=\frac{1}{\sqrt{3}}$
- Set $v_3=\frac{1}{\|\overline{v_3}\|}|\overline{v_3}\|=\begin{pmatrix}\frac{1}{\sqrt{3}}\\\frac{1}{\sqrt{3}}\\-\frac{1}{\sqrt{3}}\end{pmatrix}$. That is your third column.
You may get two different solutions (both are valid), depending on your choice of $u$ - just like in $3$-dimensional space you can have two different unit vectors orthogonal to an already given pair of orthonormal vectors. (If the two vectors are in a "horizontal" plane, the third vector may go "up" or "down".) It seems that you have one solution in your question, and I have found the other one.
In general, the Gramm-Schmidt process goes as follows: when adding a new vector to an already orthonormal set of vectors $v_1,v_2,\ldots,v_n$, you will choose $u$ to not be in the span of $v_1,v_2,\ldots,v_n$, and then you will set:
$$\overline{v_{n+1}}=u-\sum_{i=1}^n \langle u, v_i\rangle v_i$$
This will give you $\overline{v_{n+1}}$ which is already orthogonal to all of $v_1,v_2,\ldots,v_n$, but may not have the norm equal to $1$. Then you will "normalise" it:
$$v_{n+1}=\frac{1}{\|\overline{v_{n+1}}\|}\overline{v_{n+1}}=\frac{1}{\sqrt{\langle \overline{v_{n+1}},\overline{v_{n+1}}\rangle}}\overline{v_{n+1}}$$