For anyone looking to do this on Centos 7 or with another system running SystemD, you change it in
/etc/sysconfig/elasticsearch
Uncomment the ES_HEAP_SIZE line, and set a value, eg:
# Heap Size (defaults to 256m min, 1g max)
ES_HEAP_SIZE=16g
(Ignore the comment about 1g max - that's the default)