First-principle insights of initial hydration behavior affected by copper impurity in alite phase based on static and molecular dynamics calculations

Ding，Zhiheng1; Zhang，Yue1; Wang，Pan1; Wang，Muhan1; Xu，Qingqing2; Xin，Zhaorui1; Wang，Xinpeng1; Guan，Jing3; Hou，Dongshuai1

2023-04-20

10.1016/j.jclepro.2023.136478

Journal of Cleaner Production   Impact Factor & Quartile

0959-6526

1879-1786

Copper tailings have been used as a raw material for cement clinker production. The Cu element can enter into the cement phase and change its hydration behavior. In this study, the influence of Cu-doping on the structure and hydration characteristics of alite phase (tricalcium silicate, CS) are disclosed by combining the density functional theory (DFT)-based static and molecular dynamics calculations. In the static simulation, local Oi atoms move closer to doped Cu atom with Cu–O distance of 1.84–1.93 Å and forms Cu-O bonds, resulting the decrease of surface electrophilic reactivity. A single water molecule exhibits lower adsorption energies (0.92–2.12 eV) on the Cu-doped CS surface than on the pure CS surface (0.62–1.69 eV), as the chemical bonds of Ca-O and H-O were weakened. Further ab-initial molecular dynamics (AIMD) simulations cover the shortcomings of static calculations and obtain new discoveries: (a) Cu-doping promotes hydroxylation of CS surface and stabilizes fluctuation of dissociated proton. (b) Ca-O bond concentration is raised after Cu-doping, whereas the constraint effect of the CS surface on O is weakened. (c) Cu-doping accelerates the diffusion of O into water layer by ∼2 Å within 13 ps, facilitating the dissolution of clinker. These findings contribute in several ways to our understanding of the hydration properties of Cu-doping CS and provide theoretical support for the sustainable and greener development of the construction industry.

AIMD Cu-doping Tricalcium silicate Water/interface

SCI

English

Others

National Natural science foundation of China["U2006224","51978352","52008221"] ; null[ZR2020JQ25] ; null[ZR2020QE251] ; null[2019KJG010]

Science & Technology - Other Topics ; Engineering ; Environmental Sciences & Ecology

Green & Sustainable Science & Technology ; Engineering, Environmental ; Environmental Sciences

WOS:000956423300001

ELSEVIER SCI LTD

2-s2.0-85149370765

Scopus

1.Department of Civil Engineering,Qingdao University of Technology,Qingdao,China
2.Department of Ocean Science and Engineering,Southern University of Science and Technology,Shenzhen,China
3.School of Environmental and Municipal Engineering,Qingdao University of Technology,Qingdao,China

Ding，Zhiheng,Zhang，Yue,Wang，Pan,et al. First-principle insights of initial hydration behavior affected by copper impurity in alite phase based on static and molecular dynamics calculations[J]. Journal of Cleaner Production,2023,398.

Ding，Zhiheng.,Zhang，Yue.,Wang，Pan.,Wang，Muhan.,Xu，Qingqing.,...&Hou，Dongshuai.(2023).First-principle insights of initial hydration behavior affected by copper impurity in alite phase based on static and molecular dynamics calculations.Journal of Cleaner Production,398.

Ding，Zhiheng,et al."First-principle insights of initial hydration behavior affected by copper impurity in alite phase based on static and molecular dynamics calculations".Journal of Cleaner Production 398(2023).