Let me begin by saying I am slightly mistified by homology operations: I am not sure I understand them as well as I do homology cooperations and cohomology operations. Maybe someone else will be able to shine some light on them. Thankfully this is not needed in order to understand the second differential of the Atiyah-Hirzebruch spectral sequence.
I will work stably: everything in sight will be a spectrum.
It is well known and classical that cohomology operations correspond to map of spectra: that is if $E,F$ are two spectra, a natural transformation $E^*X→F^{*+n}X$ correspond by Yoneda to a map of spectra $E→\Sigma^nF$.
On the other hand if you have a map of spectra $E→\Sigma^nF$, you also get a homology operation $E_*X→F_{*-n}X$. This is because homology can be written as $$ E_*X = \pi_*(E\wedge X),\qquad F_{*-n}X=\pi_*(\Sigma^nF\wedge X)\,.$$ So understanding cohomology operations will give you also a supply of homology operations. I ignore if those are all of them (and if I had to bet I'd say no, but I cannot substantiate these feelings). This is not a dualization as you said, it is just a way to get a homology operation out of a map of spectra: no duality required.
Thankfully the second differential in the AHSS is always a homology operation of this kind. The quickest way to see this is by looking at the construction of the AHSS that uses the Postnikov tower for the spectrum $E$ instead than the one using the cellular filtration for $X$ (this will also show that the differential $d_2$ correspond essentially to the k-invariants of $E$). That is, we can look at the AHSS as the spectral sequence associated to the exact couple
$$\require{AMScd} \begin{CD} \dots @>>> \pi_*(P_{n+1}E\wedge X) @>>> \pi_*(P_nE\wedge X) @>>> \pi_*(P_{n-1}E\wedge X) @>>> \cdots\\ {} @VVV {} @VVV {} @VVV {}\\ \dots @. \pi_*(H\pi_{n+1}E \wedge X)=H_*(X;\pi_{n+1}E) @. \pi_*(H\pi_nE\wedge X)=H_*(X;\pi_nE) @. \pi_*(H\pi_{n-1}E\wedge X)=H_*(X;\pi_{n-1}E) @.\cdots \end{CD}$$
That is the $d_2:H_*(X;\pi_nE)\to H_{*-1}(X;\pi_{n+1}E)$ is induced by the map of spectra $$H\pi_nE\to \Sigma P_{n+1}E\to \Sigma H\pi_{n+1}E\,.$$ So we can leverage our understanding of the cohomology operations to get at the $d_2$ of the AHSS.
Now let us tackle homology cooperations. These are the homotopy classes of $E\wedge E$. I really do not have too much to say about them: they show up because they are important for the Adams spectral sequence (in fact they basically run the show there). They are also the "dual" of the cohomology operations. If $E$ is an $E_\infty$-ring spectrum we can use the universal coefficient spectral sequence to go $$\mathrm{Ext}_{E_*}(\pi_*(E\wedge E),E_*) \Rightarrow \pi_*F_E(E\wedge E,E)=\pi_*F(E,E)$$ where $F_E$ and $F$ are the internal hom in $E$-modules and spectra respectively. For example when $E=Hk$ for $k$ a field (the main case people treat I think) this spectral sequence degenerates telling you that the $k$-linear dual of $\pi_*(Hk\wedge Hk)$ is the ring of cohomology operations. As you can see these have no direct relation to homology operations and they arise in a different setting altogether.
Finally, the Hurewicz homomorphism. This is, by definition, the map on homology theories defined by the map $h:\mathbb{S}\to H\mathbb{Z}$ sending 1 to 1. In fact, if $f:\Sigma^n\mathbb{S}\to X$ is a class in $\pi_nX$ we are sending it to the image of the fundamental homology class of $\Sigma^n\mathbb{S}$. But the fundamental homology class is just the map $$\Sigma^nh=(h\wedge 1):\Sigma^n\mathbb{S}\to H\mathbb{Z}\wedge\Sigma^n\mathbb{S}\,.$$ So we are sending $f$ to $(1_{H\mathbb{Z}}\wedge f)\circ (h \wedge 1) = (h\wedge f)$, that is we are doing the homology operation represented by $h$.