Sulfidated zero-valent iron (S-ZVI) enhances the degradation of chlorinated hydrocarbon (CHC) in contaminated groundwater. Despite numerous studies of S-ZVI, a versatile strategy to improve its dechlorination kinetics, electron efficiency (ε e ), and dechlorination capacity is still needed. Here, we used heteroatom incorporation of N(C) and S by ball-milling of microscale ZVI with melamine and sulfur via nitridation and sulfidation to synthesize S-N(C)-mZVI bm particles that contain reactive Fe-N X (C) and FeS species. Sulfidation and nitridation synergistically increased the trichloroethene (TCE) dechlorination rate, with reaction constants k SA of 2.98 × 10 −2 L•h −1 •m −2 by S-N(C)-mZVI bm , compared to 1.77 × 10 −3 and 8.15 × 10 −5 L•h −1 •m −2 by S-mZVI bm and N(C)-mZVI bm , respectively. Data show that sulfidation suppressed the reductive dissociation of N(C) from S-N(C)-mZVI bm , which stabilized the reactive Fe-N X (C) and reserved electrons for TCE dechlorination. In addition to lowering H 2 production, S-N(C)-mZVI bm dechlorinated TCE to less reduced products (e.g., acetylene), contributing to the material's higher ε e and dechlorination capacity. This synergistic effect on TCE degradation can be extended to other recalcitrant CHCs (e.g., chloroform) in both deionized and groundwater. This multiheteroatom incorporation approach to optimize ZVI for groundwater remediation provides a basis for further advances in reactive material synthesis.

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