2026-10-14T05:12:46Z https://api.figshare.com/v2/oai

oai:figshare.com:article/34033398 2026-09-30T15:15:42Z category_146 category_24 category_272 category_873 category_39 category_734 portal_63 item_type_6 month_year_09_2026

Regulating Localized Proton Delivery in CuCo-LDH@TiO₂ Heterojunctions for Selective Photocatalytic Nitrate Hydrogenation Xing’an Dong (8990684) Yuying Wang (532738) Xian Shi (1914337) Chen Yang (207381) Tianyao Ren (25144635) Weidong Dai (135643) Wendong Zhang (1302618) Peng Yu (48605) Guangming Jiang (1477540) Fan Dong (454080) Space Science Evolutionary Biology Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified Ecology Biological Sciences not elsewhere classified primary hydrogen reservoir optimized nominal 3 nearly quantitative nh general design paradigm derived hydrogen available coordinating paired half 86 ± 0 proposed interfacial proton kinetically accessible supply couple nitrate removal couple nitrate reduction local hydrogen supply derived proton equivalents 2 </ sub proton equivalents local supply nitrate conversion work demonstrates tested conditions tailoring oxidation structure calculations side chemistry product analysis peroxide chemistry oxidation chemistry isotope measurements hcho oxidation forms hcooh equivalent relay effectively regulate ammonia recovery Photocatalytic nitrate reduction can couple nitrate removal with ammonia recovery. Successive hydrogenation steps require a local supply of proton equivalents, but making water-derived hydrogen available at nitrate-reduction sites remains difficult. Here, CuCo-LDH supported on anatase TiO₂ nanosheets (CuCo-LDH@TNS) is constructed to couple nitrate reduction with water/peroxide chemistry and HCHO oxidation. The optimized nominal 3% CuCo-LDH@TNS catalyst gives 94.86 ± 0.66% nitrate conversion and nearly quantitative NH₄⁺ selectivity. Spectroscopic and isotope measurements, together with product analysis and electronic-structure calculations, support a proposed interfacial proton-equivalent relay. HCHO consumes oxidation equivalents and forms HCOOH/formate, while water remains the primary hydrogen reservoir under the tested conditions. The heterointerface therefore couples nitrate reduction on CuCo-LDH with oxidation chemistry on TNS, maintaining a kinetically accessible supply of water-derived proton equivalents. This work demonstrates that tailoring oxidation-side chemistry can effectively regulate the local hydrogen supply, offering a general design paradigm for coordinating paired half-reactions toward selective green ammonia synthesis. 2026-09-30T00:00:00Z Text Journal contribution 10.1021/acsnano.6c12813.s001 https://figshare.com/articles/journal_contribution/Regulating_Localized_Proton_Delivery_in_CuCo-LDH_TiO_sub_2_sub_Heterojunctions_for_Selective_Photocatalytic_Nitrate_Hydrogenation/34033398 CC BY-NC 4.0