Cellulose nanocrystals (CNC) and nanofibers (CNF) have been broadly studied as renewable nanomaterials for various applications, including additives in cement and plastics composites. Herein, life cycle inventories for 18 previously examined processes are harmonized, and the impacts of CNC and CNF production are compared with a particular focus on GHG emissions. Findings show wide variations in GHG emissions between process designs, from 1.8-1100 kg CO2-eq/kg nanocellulose. Mechanical and enzymatic processes are identified as the lowest GHG emission methods to produce CNCs and CNFs. For most processes, energy consumption and chemical use are the primary sources of emissions. However, on a mass basis, for all examined production methods and impact categories (except CO emissions), CNC and CNF production emissions are higher than Portland cement and, in most cases, are higher than polylactic acid. This work highlights the need to carefully consider process design to prevent potential high emissions from CNCs and CNF production despite their renewable feedstock, and results show the magnitude of conventional material that must be offset through improved performance for these materials to be environmentally favorable.

The pyroclastic aggregate concrete of Trajan's Markets (110 CE), now Museo Fori Imperiali in Rome, has absorbed energy from seismic ground shaking and long-term foundation settlement for nearly two millenia while remaining largely intact at the structural scale. The scientific basis of this exceptional service record is explored through computed tomography of fracture surfaces and synchroton X-ray microdiffraction analyses of a reproduction of the standardized hydrated lime-volcanic ash mortar that binds decimeter-sized tuff and brick aggregate in the conglomeratic concrete. The mortar reproduction gains fracture toughness over 180 d through progressive coalescence of calcium-aluminum-silicate-hydrate (C-A-S-H) cementing binder with Ca/(Si+Al) ≈ 0.8-0.9 and crystallization of strätlingite and siliceous hydrogarnet (katoite) at ≥ 90 d, after pozzolanic consumption of hydrated lime was complete. Platey strätlingite crystals toughen interfacial zones along scoria perimeters and impede macroscale propagation of crack segments. In the 1,900-y-old mortar, C-A-S-H has low Ca/(Si+Al) ≈ 0.45-0.75. Dense clusters of 2- to 30-µm strätlingite plates further reinforce interfacial zones, the weakest link of modern cement-based concrete, and the cementitious matrix. These crystals formed during long-term autogeneous reaction of dissolved calcite from lime and the alkali-rich scoriae groundmass, clay mineral (halloysite), and zeolite (phillipsite and chabazite) surface textures from the Pozzolane Rosse pyroclastic flow, erupted from the nearby Alban Hills volcano. The clast-supported conglomeratic fabric of the concrete presents further resistance to fracture propagation at the structural scale.