Conversion of dinitrogen to ammonia by FeN 3 -embedded
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1 SUPPLEMENTARY MATERIAL FOR Conversion of dinitrogen to ammonia by FeN 3 -embedded Graphene Xiao-Fei Li 1, *, Qin-Kun Li 1, Jin Cheng 1, Lingling Liu 1, Qing Yan 1, Yingchao Wu 1, Xiang-Hua Zhang 1, Zhi-Yong Wang 1, Qi Qiu 1, and Yi Luo 2 1 School of Optoelectronic Information, University of Electronic Science and Technology of China, Chengdu, Sichuan, , China 2 Hefei National Laboratory for Physical Sciences at the Microscale and Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui , China * xf.li@uestc.edu.cn Figure S1. Two structures: (a) FeN 3 -graphene and (b) FeN 4 -graphene are considered. The vacuum thickness between graphene layers was set as 15 Å to avoid inter-layer interaction. A single and a double vacancy (SV, DV) of the graphene formed by threeand four-nitrogen-atom doping graphene (N x -graphene, x=3,4) were used for confining the Fe site, respectively. All the calculations were carried out by means of S1
2 spin-resolved density functional theory (DFT) including vdw corrections (vdw-dft) as implemented in Vienna Ab initio Simulation Package (VASP-5.3). The projector augmented wave (PAW) pseudo-potential was used to describe the core electrons, and a 500 ev cutoff energy for the plane-wave basis set was used for the valence electrons. The revised Perdew-Burke-Ernzerhof (rpbe) generalized gradient approximation (GGA) was chosen for the exchange correlation potential. The grids of were used for the k-point meshes in the first Brillouin zone (BZ) of the supercell. The total spin was not fixed during the structural optimization, and the optimization stopped until the residual force on each atom was smaller than ev Å -1. The triplet or quintet states were considered in the unrestricted (spin-polarized) framework. The structure of the minimum energy was used for relative calculations. And the lowest energy of the triplet (quintet) state, singlet state and non-polarized state was used for energy-related calculations. Considered the Mulliken charges are not so reliable when plane wave basis set is used. The Mulliken charges are obtained in SIESTA 3.2 1, using double-ζ polarization basis sets (DZP). Test calculations show that the cutoff energy increasing up to 700 ev changed the bonding energy by less than 10 mev for FeN 3 -graphene, and the same accuracy was achieved with respect to the k-point meshes over the BZ grids up to S2
3 Figure S2. The optimized structures of the intermediates in the distal, alternating, enzymatic reaction pathway. Each step is modeled as the scheme of Figure 3. For clarity, the graphene is not shown. Table S1. The N-N bond length (Å) of the adsorbed N 2 in the three reaction pathways (distal, alternating, enzymatic pathway, respectively) step Free N distal alternating enzymatic S3
4 Table S2. The spin moment (µ B ) of intermediates in each step of the distal, alternating, enzymatic reaction pathway, respectively, as shown in Figure 3. For clarity, the N 3 G moiety is omitted, such as: Fe N N represents (N 3 G)Fe N N. intermediates distal intermediates alternating intermediates enzymatic Fe N N 3.27 Fe N N 3.27 Fe(N N) 3.13 Fe N NH 2.19 Fe N NH 2.19 Fe(N NH) 3.05 Fe N NH Fe NH NH 3.36 Fe(HN NH) 4.03 Fe N NH Fe NH NH Fe(HN NH 2 ) 3.14 Fe NH 3.19 Fe NH 2 NH Fe(H 2 N NH 2 ) 3.96 Fe NH Fe NH 2 NH Fe(H 2 N NH 3 ) 3.08 Fe NH Fe NH Fe NH Table S3. The reaction energies ( E, ev) in each step of the distal, alternating, enzymatic reaction pathway, respectively, as shown in Figure 3. For clarity, the energy of the (N 3 G)Fe is set to be energy benchmark(0 ev). And the step 0 means the adsorption of N 2, which differ from the Figure 3. Reaction steps distal alternating enzymatic (N 3 G)Fe S4
5 Table S4. Variation of Mulliken charge (the charge difference of the present step from that of the previous step) of the three moieties (shown in Figure 5) in the catalyst of the distal, alternating, enzymatic reaction pathway, respectively, as shown in Figure 3. The step 0 means the adsorption of N 2 and step 7 means the release of NH 3, which differ from the Figure 3. And the 1, 2, 3 means the moiety1, moiety2, moiety3, respectively. reaction steps distal alternating enzymatic Table S5. The energies in hartrees of some optimized structures which are in ferromagnetic states. The N 3 G and N 4 G in following structural formulas means threeand four-nitrogen-atom doping graphene (N x -graphene, x=3,4) shown in Figure S1. intermediates energies intermediates energies N N 3 G Fe(atomic) (N 3 G)Fe Fe(in bulk) (N 3 G)Fe N N N 4 G (N 3 G)Fe(N N) (N 4 G)Fe (N 3 G)Fe N NH (N 4 G)Fe N N (N 3 G)Fe(N NH) S5
6 Table S6. Geometrical coordinates of the optimized structures of some intermediates for electronic structure calculations. Note: fast links to the coordinates of following intermediates (please hold down the CTRL key and click the mouse on the target field for quick access) N 4 G (N 4 G)Fe (N 4 G)Fe N N N 3 G (N 3 G)Fe (N 3 G)Fe N N (N 3 G)Fe(N N) (N 3 G)Fe N NH (N 3 G)Fe(N NH) N 4 G Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S6
7 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C N N N N (N 4 G)Fe S7
8 Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S8
9 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C N N N N Fe (N 4 G)Fe N N Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C S9
10 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S10
11 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C N N N N N N Fe N 3 G Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S11
12 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S12
13 C C C C C C N N N (N 3 G)Fe Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S13
14 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C N N N Fe (N 3 G)Fe N N Atoms X Y Z C C C C C C C C C C C S14
15 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S15
16 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C N N N Fe N N (N 3 G)Fe(N N) Atoms X Y Z C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S16
17 C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C C S17
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