The cause is theobromine, a poison similar to caffeine(and which despite its name does not contain Bromine). The effect is caused by a combination of low body mass, inefficient metabolic processes and for dogs the tendency to indiscriminately eat random things. The low body mass means its a lot easier to find enough of the stuff. a bar of chocolate might kill a 5kg dog but wont bother a 1ton cow. The inefficient metabolism means its about 4 times more poisonous to cats and dogs than it is to humans or rats. And the indiscriminate eating means a dog can eat more chocolate than a human, despite being smaller.
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