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FUEL · 2025 · IF 7.5

Identification of active sites for formaldehyde oxidation on mesoporous Pt/CeO2 catalyst at ambient temperature and low humidity

Ruichen Wang,Chao Yu,Juanjuan Gong,Qingfa Su,Hui Chen,Canyan Yang,Shaodi Sun,Zhiwei Huang,Huazhen Shen,Huawang Zhao,Bihong Lv,Xiaomin Wu,Guohua Jing

Identification of active sites governing the performance of indoor formaldehyde (HCHO) oxidation at ambient temperature and low humidity is crucial for developing improved catalysts, but remains challenging. It has recently been discovered that the effective dissociation of water is of importance for HCHO oxidation at low humidity. Here, we have elaborately designed a Pt supported on three-dimensionally ordered mesoporous CeO 2 catalyst (Pt/kit-CeO 2 ). The Pt/kit-CeO 2 catalyst achieves ∼ 95 % CO 2 yield for a long time. The results indicate that the abundant oxygen vacancies and single coordination-unsaturated Ce sites on mesoporous CeO 2 enhance H 2 O dissociation, leading to the generation of a substantial amount of terminal hydroxyl groups (OH t ). These OH t groups promote the oxidation of intermediate dioxymethylene (DOM) and formate species, thereby regulating the catalytic activity. Additionally, the dispersed Pt facilitates the activation of O 2 , generating active oxygen species (O*) that work synergistically with OH t groups to promote the conversion of formates into CO 2 . The in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) further elucidated the mechanism of catalyst promoting HCHO oxidation: HCHO (+O*) → DOM (+OH t ) → HCOO – /HCOOH (+OH t /O*) → CO 3 2– → CO 2 . We anticipate that this knowledge will inspire the development of Pt-based catalysts specifically tailored for low humidity.

CAS / MDL: 1306-38-3
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Unsaturated NiO Incorporated PtNi, Possessing Abundant Surface Hydroxyl Species, as an Efficient and Durable Electrocatalyst for the Hydrogen Evolution Reaction in Seawater

Xiong Yang,Lu Wu,Yi-Yuan Wang,Bing-Bing Jia,Yu-Xuan Xiao,Ge Tian,Jie Ying,Yi Lu,Si-Ming Wu,Wei Geng,Fei Yu,Ling Shen,Ion Tiginyanu,Xiao-Yu Yang

Creating an abundance of OH * active sites on the surface of an electrocatalyst is an ideal approach for improving both its performance and Cl – corrosion resistance in seawater splitting to generate hydrogen via the hydrogen evolution reactions (HER). However, the development of strategies for designing coordinatively saturated metals that have these sites remains a significant challenge. Herein, we report on the development of NiO/Pt 3 Ni-300, a coordinatively unsaturated NiO incorporated Pt 3 Ni, which has the ability to capture large numbers of surface hydroxyl groups during the HER in seawater and, in consequence of this, it exhibits high electrocatalytic activity in seawater. Additionally, benefiting from super-hydrophilicity induced by its rich OH * surface, NiO/Pt 3 Ni-300 preferentially adsorbs H 2 O over Cl – . The outstanding HER performance of this catalyst in alkaline seawater is reflected by a low overpotential of 16 mV to drive a current density of 10 mA cm −2 , and a 7.7-fold higher turnover frequency compared to that of Pt/C. Moreover, it displays only a small 41 mV drop in overpotential after promotion of the HER for 20 h in alkaline seawater, a value that surpasses those inherent to commercial Pt/C, Pt 3 Ni, and crystalline NiO incorporated Pt 3 Ni.

CAS / MDL: 16941-12-1 7718-54-9
研究领域: 电催化 · 能源材料 · 氢气制备 · 可再生能源 · 材料化学
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Nature Communications · 2024 ·Vol. 15 ·期 1 ·1-17 · IF 14.7

Understanding the active site in chameleon-like bifunctional catalyst for practical rechargeable zinc-air batteries

Zhong Xiongwei,Xiao Xiao,Li Qizhen,Zhang Mengtian,Li Zhitong,Gao Leyi,Chen Biao,Zheng Zhiyang,Fu Qingjin,Wang Xingzhu,Zhou Guangmin,Xu Baomin

The practical application of rechargeable zinc-air batteries faces challenges stemming from inadequate bifunctional catalysts, contradictory gas-liquid-solid three-phase interfaces, and an ambiguous fundamental understanding. Herein, we propose a chameleon-like bifunctional catalyst comprising ruthenium single-atoms grafted onto nickel-iron layer double hydroxide (Ru SA -NiFe LDH). The adaptive oxidation of Ru SA -NiFe LDH to oxyhydroxide species (Ru SA -NiFeOOH) during charging exposes active sites for the oxygen evolution reaction, while reversible reduction to NiFe LDH during discharge exposes active sites for the oxygen reduction reaction. Additionally, a hierarchical air cathode featuring hydrophilic and hydrophobic layers facilitates the reversible conversion between Ru SA -NiFe LDH and Ru SA -NiFeOOH, expedites oxygen bubble desorption, and suppresses carbon corrosion. Consequently, our zinc-air batteries demonstrate a high charge/discharge capacity of 100 mAh cm −2 per cycle, a voltage gap of 0.67 V, and an extended cycle life of 2400 h at 10 mA cm −2 . We comprehensively elucidate the catalytic reaction thermodynamics and kinetics for the air cathode through electrode potential decoupling monitoring, oxygen bubble desorption tracking, and carbon content quantification.

研究领域: 材料科学 · 电化学 · 能源存储
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