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It is not possible to take a screenshot by holding both volume buttons on the PinePhone. The ADC driver in the device can only send one keypress at a time, so we cannot know when both buttons are pressed.

A possible solution to this is using Power+Volume (up or down) to take a screenshot.

In the mean time, you can add a button to the Shell for taking a screenshot. Add the following to the end of the Shell.qml file, but before the final closing brace:

    Button {
        color: "white"
        text: "Screenshot"
        anchors {
            bottom: parent.bottom
            right: parent.right
        }
        onClicked: itemGrabber.capture(shell)
    }