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Development of a Reactive Force Field for Simulations on the Catalytic Conversion of C/H/O Molecules on Cu-Metal and Cu-Oxide Surfaces and Application to Cu/CuO-Based Chemical Looping

Summary

A Cu/C/H/O Reaxff is built by re-optimizing Cu on cluster data, merging with a C/H/O field, and fitting Cu–(C/H/O) cross-terms to DFT binding and barriers on Cu(100), (111), (211). Custom Reaxff-based transition-state and reaction-path utilities are presented. LAMMPS NVT reactive MD ( Berendsen thermostat, 0.1 ps damping) at 600–1600 K and 0.25 fs covers H dissociation, methoxy chemistry, glucose + Cu at 1600 K ( 400 ps gas leg), and CLC-style redox tours (Section 3; SI for cell sizes).

This slug is an alternate PDF path (online file name) for the same DOI as [[2020wenbo-zhu-j-phys-chem-jp0c02573]].

Methods

1 — MD application. LAMMPS; NVT; Berendsen thermostat; 0.25 fs time step; temperature setpoints in 600–1600 K (e.g. 600 K, 1000 K, 1400 K, 1600 K for the illustrative cases in Section 3); trajectory durations include 400 ps for the glucose gas-phase leg and other ps-scale production segments in Section 3; PBC slabs with ~10–20 Å vacuum as in SI. N/A — NPT; N/A — umbrella; N/A — E-field. Hydrostatic pressure N/A under NVT sampling in the examples quoted here.

2 — Force-field training. Reoptimize Cu; merge C/H/O; fit cross-terms to DMol3 rPBE data (energies, barriers); see [[2020wenbo-zhu-j-phys-chem-jp0c02573]] for full DFT convergence ladder.

3 — Static QM. DMol3 rPBE; LST/QST/CG for TS; identical to the VOR curation on the primary wiki page.

4 — Review or non-simulation. N/A

Findings

Outcomes and mechanisms. DFT-consistent surface chemistry and rich C/H/O MD on Cu; fuel-dependent CLC outcomes when O storage on CuO couples to fragmentation on Cu (facets), as framed in the full text.

Comparisons and sensitivity. Reaxff vs DFT on adsorption/barriers; T sweeps; case-by-case chemistry (methoxy, glucose, hydrocarbons).

Authored limitations and outlook. Transferability to electrochemical interfaces with explicit electrolyte may need more training—see ## Limitations below.

Corpus honesty. Provenance of this file = second PDF name; use the VOR file for page-stable citations if pagination drifts between preprint/ Just-Accepted/ VOR builds (confirm in PDF).

Limitations

Transferability to electrolyte-covered Cu under electrochemical control is not automatic; explicit solvation and charged interfaces may need additional training. Corpus operators should treat combustion and CLC case studies as illustrative trajectories whose statistics (barrier sampling, long runtime needs) must be read from the VOR PDF and SI tables, not inferred from this navigation slug** alone.

Relevance to group

van Duin co-authorship; parameterization + method tooling (TS search) for metal oxidation/catalysis.

Citations and evidence anchors

  • DOI: 10.1021/acs.jpcc.0c02573

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