We report the first use of polymeric carbon nitride (CN) for the catalytic selective oxidation of HS. The as-prepared CN with unique ultrathin "nanomeshes" structure exhibits excellent HS conversion and high S selectivity. In particular, the CN nanomesh also displays better durability in the desulfurization reaction than traditional catalysts, such as carbon- and iron-based materials.

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A series of graphitic carbon nitride (CN) in the form of nanosheets with porous structure have been prepared through thermal treatment of bulk CN in air. Compared with the bulk counterpart, the as-generated holey CN nanosheets are larger in specific surface area. Endowed with more active sites and enhanced mass transport ability, the latter display catalytic performance substantially superior to the former, exhibiting higher H2S conversion and S selectivity in the oxidation of H2S to S. Moreover, the CN nanosheets show much better durability than traditional catalysts. It is envisaged that the strategy is a general technique that can be extended to produce porous CN nanosheets from other nitrogen-rich precursors, as well as to prepare other 2D carbon-based materials for potential applications.

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Iron‐based catalysts have been widely studied for the oxidation of H2S into elemental S. However, the prevention of iron sites from deactivation remains a big challenge. Herein, a facile copolymerization strategy is proposed for the construction of isolated Fe sites confined in polymeric carbon nitride (CN) (Fe‐CNNχ). The as‐prepared Fe‐CNNχ catalysts possess unique 2D structure as well as electronic property, resulting in enlarged exposure of active sites and enhancement of redox performance. Combining systematic characterizations with density functional theory calculation, it is disclosed that the isolated Fe atoms prefer to occupy four‐coordinate doping configurations (Fe–N4). Such Fe–N4 centers favor the adsorption and activation of O2 and H2S. As a consequence, Fe‐CNNχ exhibit excellent catalytic activity for the catalytic oxidation of H2S to S. More importantly, the Fe‐CNNχ catalysts are resistant to water and sulfur poisoning, exhibiting outstanding catalytic stability (over 270 h of continuous operation), better than most of the reported catalysts.

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Efficient catalytic elimination of hydrogen sulfide (H2S) with high activity and durability in nature gas and blast‐furnace gas is very critical for both fundamental catalytic research and applied environmental chemistry. Herein, atomically dispersed Co atom catalysts with Co–N4 sites that can transform H2S into S with conversion rate of ≈100% are designed and prepared. The representative 4Co‐N/NC achieves a sulfur yield of nearly 100% and TOF(Co) of 869 h–1 at 180 °C. Importantly, remarkable long‐term durability is achieved as well, with no obvious loss of catalytic activity in the run of 460 h, outperforming most of the reported catalysts. The short bond length and strong cooperation of Co–N are beneficial to improve the structural stability of the Co–N4 centers, and significantly enhanced resistance of water and sulfation over single‐atom Co‐catalyst. The present mechanism involves the stepwise hydrogen transfer process via the adsorbed *HOO and *HS intermediates.