Zhi-Wei Sun introduced this sequence in arXiv:1407.0967. For any prime p > 5, he proved that Sum_{k=1..p-1} a(k)/k^2 == 0 (mod p) and Sum_{k=1..p-1} a(k)/k == 0 (mod p^2). This is quite similar to Wolstenholme's congruences Sum_{k=1..p-1} 1/k^2 == 0 (mod p) and Sum_{k=1..p-1} 1/k == 0 (mod p^2) for any prime p > 3.
Conjecture: For any prime p > 5 and positive integer n, the number (a(p*n) - a(n))/(p*n)^3 is always a p-adic integer.
The author proved a weaker version of this in arXiv:1610.03384. - Zhi-Wei Sun, Nov 12 2016
Conjecture: a(n) = Sum_{k = 0..n} binomial(n, k)*b(k), where b(n) = Sum_{k = 0..n} (-1)^k*binomial(n, k)^2*binomial(2*k, n). [Added Mar 16 2025: this conjecture can be verified using the MulZeil procedure in Doron Zeilberger's MultiZeilberger package for Maple]. - Peter Bala, Jul 19 2024