If you want to raise the button's Click event programmatically when the + key is pressed, you could handle the KeyDown event of the form:
public partial class Form1 : Form
{
public Form1()
{
InitializeComponent();
this.KeyPreview = true;
this.KeyDown += Form1_KeyDown;
}
void Form1_KeyDown(object sender, KeyEventArgs e)
{
if (e.KeyCode == Keys.Oemplus)
{
buttonAdd.PerformClick();
}
}
private void buttonAdd_Click(object sender, EventArgs e)
{
//handle click...
}
}