Preparation of phosphorus-doped tungsten trioxide nanomaterials and their photocatalytic performances

Sun, Jiayu; Li, Bihan; Wang, Qi; Zhang, Ping; Zhang, Yulei; Li, Xiaochen

doi:10.1080/09593330.2020.1745292

Cited by 15 publications

(1 citation statement)

References 33 publications

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“…To fabricate P-OV-WO 3 , a gas–solid phase reaction approach was developed to avoid contamination of the surface of final products. − Briefly, red phosphorus and tungstic acid (H 2 WO 4 or WO 3 ·H 2 O) nanosheets were selected as the doping source and precursor, respectively. The H 2 WO 4 nanosheets were first fabricated via a hydrothermal method with a slightly modified protocol as described in Supporting Information S1 .…”

Section: Methodsmentioning

confidence: 99%

Enhancement of Electrochemical Nitrogen Reduction Activity and Suppression of Hydrogen Evolution Reaction for Transition Metal Oxide Catalysts: The Role of Proton Intercalation and Heteroatom Doping

Li,

Kucukosman,

et al. 2024

ACS Catal.

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During the electrochemical nitrogen reduction reaction (eNRR) and hydrogen evolution reaction (HER), interstitial proton intercalation readily occurs in some transition metal oxide (TMO) catalysts and changes their d-band electronic structure. This work fabricated phosphorus (P)-doped tungsten oxide (WO 3 ) with enriched oxygen vacancies (OVs) to study the impact of proton intercalation and heteroatom doping on eNRR and HER. Our results demonstrated that the electronic structure of the P-OV-WO 3 catalyst was altered by in situ proton intercalation as indicated by the greater negative onset potential of eNRR at −0.05 V compared to the proton intercalation potential of 0.3 V versus reversible hydrogen electrode (RHE). Compared to the non-P-doped WO 3 , the introduction of P doping in WO 3 (e.g., 4.8 at. %) led to a reduction of more than 36% in proton intercalation. As a result, the HER activity of the P-OV-WO 3 was significantly suppressed, as demonstrated by a considerably negative shift of the onset HER potential from −0.06 to −0.15 V and a slower HER kinetics with the Tafel slope increased from 129.0 to 343.1 mV/dec. Density functional theory calculations revealed the synergy of the proton intercalation, substitutional P doping, and the associated OVs in the improvement of N 2 activation and hydrogenation in eNRR. The increased eNRR and the suppressed HER led to a high Faradaic efficiency (FE) of 64.1% and the NH 3 yield of 24.5 μg• mg cat −1 h −1 at −0.15 V versus RHE in H 2 SO 4 (pH = 2) as the electrolyte. The specific NH 3 yield is more than 20 times higher than that of C-WO 3 (1.1 μg•mg cat −1 h −1 with a FE of 20%). The results exceed most of the reported eNRR performances for TMO-based catalysts. Thus, the synergistic proton intercalation and P doping could lead to newer designs and applications of TMO-based catalysts for improved eNRR while suppressing the competing HER.

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