The correct option is D although they supplemented
The error in the sentence, here, is in the parallel structure (one sentence structure where there is a list or series of items or actions separated by commas). The sentence structure is like - subject + verb, but verb, where the two verbs need to be parallel to each other. In option A, 'supplementing' becomes a progressive participle whereas the sentence is in simple past tense ('were'). Thus, option A is incorrect as it does not make for a correct parallel structure. E is also incorrect for similar reason where there's a prepositional phrase that acts as a gerund. Though 'and' fits into a parallel structure, it does not convey the contrast that's required in this context. This is one of the reasons why B is incorrect. The other reason being the failure of past perfect tense 'had supplemented' as a parallel structure since the sentence is in simple past ('were'). C is grammatically incorrect because along with the use of 'and', there's a subordinate clause 'even though...' and it seems as if the 'and' is left hanging while we wait for another Independent clause. Thus D is the only option that befits the context- 'although' provides the contrast required and it complies with the demands of a parallel structure.