There are areas in the country I live in where deforestation has been extreme. I'm thinking of going to transplant smaller trees from the neighboring forests.
Does this make sense? Could I end up doing more harm than good?
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By moving a tree from one area to another, that's -1 tree to the source and +1 tree to the destination, for a net change of 0 trees over the region. That probably won't make much of a difference overall. The specific tree being moved might fare slightly better or worse over its lifetime, which could have a small impact, good or bad.
Maybe the real question here is about the best (or fastest) method of afforestation. Is it best to plant trees from seed, or transplant saplings, or something else? Large-scale afforestation sometimes has problems (like planting too many of a single species of tree, all at the same age) but perhaps introducing seedlings and saplings of various species and age might better contribute to the re-development of forest biodiversity. I'm not an expert here, so hopefully a real forest scientist can provide a better answer.
I think you'll find that in areas where forests are managed, baby trees come from a central location the only purpose of which is to grow lots of these small baby trees.
The trees are used to create a new forest in an area where the old forest has been cut down for timber.
In contrast to letting the new forest be naturally seeded, obtaining the baby trees from the central location where only the trees with the best genes are grown, you obtain better genes for the trees. The trees in the forest grow faster than they would grow if the forest was naturally seeded.
So, the answer to:
Would moving baby trees help with carbon sequestration?
YES, and it is currently being done in massive scale in countries with managed forest (example: Finland).