“…To circumvent this, composite materials including high-surface-area porous carbon ( Collins, 2014 ; Collins et al., 2018 , 2015 ; 2014 , 2013 ; Ferrari and Robertson, 2000 ), core-shell-type powder or slurry silicon additives ( Chae et al., 2020 ; Guo et al., 2017 ; Hu et al., 2008 ; Jia et al., 2018 ; Vrankovic et al., 2017 ; Wang et al., 2013 ; Xing et al., 2018 ; Xu et al., 2018 ; Zhai et al., 2017 ), or porous silicon (PS) ( An et al., 2019 ; Chen et al., 2019 ; Gardner et al., 2016 ; Ikonen et al., 2017 ; Jia et al., 2018 ; Karbassian, 2018 ; Lu et al., 2015b ; Xiao et al., 2015 ) have been in constant development. PS-based systems, in particular, yield opportunities for advanced control of Li-diffusion and plating processes through the manipulation of internal silicon-charge dynamics, where crystal structure can be formidably tuned by select surface functional groups ( Buttard et al., 1996 ; Ghannam et al., 2008 ; Sugiyama and Nittono, 1990 ) enabling enhancement of reversible electrochemical processes. Such surface-to-bulk structure/function relationships have been well elucidated via functional groups on high-surface-area carbon ( Collins, 2014 ; Collins et al., 2018 , 2015 , 2014 , 2013 ), thereby presenting an even greater opportunity for desired electrode performance when utilizing silicon with an additional filled π-orbital within Group 14 of the periodic table.…”