Nature Communications
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2024
·Vol. 15
·期 1
·1-9
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IF 14.7
Sun Jikai,Tu Rui,Xu Yuchun,Yang Hongyan,Yu Tie,Zhai Dong,Ci Xiuqin,Deng Weiqiao
The process of CH 4 cracking into H 2 and carbon has gained wide attention for hydrogen production. However, traditional catalysis methods suffer rapid deactivation due to severe carbon deposition. In this study, we discover that effective CH 4 cracking can be achieved at 450 °C over a Re/Ni single-atom alloy via ball milling. To explore single-atom alloy catalysis, we construct a library of 10,950 transition metal single-atom alloy surfaces and screen candidates based on C–H dissociation energy barriers predicted by a machine learning model. Experimental validation identifies Ir/Ni and Re/Ni as top performers. Notably, the non-noble metal Re/Ni achieves a hydrogen yield of 10.7 gH 2 gcat –1 h –1 with 99.9% selectivity and 7.75% CH 4 conversion at 450 °C, 1 atm. Here, we show the mechanical energy boosts CH 4 conversion clearly and sustained CH 4 cracking over 240 h is achieved, significantly surpassing other approaches in the literature.
研究领域:
催化化学
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材料科学
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能源科学
✓ 已验证
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
·
IF 14.7
Wang Shifu,Li Fuhua,Zhao Jian,Zeng Yaqiong,Li Yifan,Lin Zih-Yi,Lee Tsung-Ju,Liu Shuhui,Ren Xinyi,Wang Weijue,Chen Yusen,Hung Sung-Fu,Lu Ying-Rui,Cui Yi,Yang Xiaofeng,Li Xuning,Huang Yanqiang,Liu Bin
Manipulation C-C coupling pathway is of great importance for selective CO 2 electroreduction but remain challenging. Herein, two model Cu-based catalysts, by modifying Cu nanowires with Ag nanoparticles (AgCu NW) and Ag single atoms (Ag 1 Cu NW), respectively, are rationally designed for exploring the C-C coupling mechanisms in electrochemical CO 2 reduction reaction (CO 2 RR). Compared to AgCu NW, the Ag 1 Cu NW exhibits a more than 10-fold increase of C 2 selectivity in CO 2 reduction to ethanol, with ethanol-to-ethylene ratio increased from 0.41 over AgCu NW to 4.26 over Ag 1 Cu NW. Via a variety of o perando /in-situ techniques and theoretical calculation, the enhanced ethanol selectivity over Ag 1 Cu NW is attributed to the promoted H 2 O dissociation over the atomically dispersed Ag sites, which effectively accelerated *CO hydrogenation to form *CHO intermediate and facilitated asymmetric *CO-*CHO coupling over paired Cu atoms adjacent to single Ag atoms. Results of this work provide deep insight into the C-C coupling pathways towards target C 2+ product and shed light on the rational design of efficient CO 2 RR catalysts with paired active sites.
研究领域:
材料科学
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电化学
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Energy
·
2025
·
IF 17.1
Peng Bai,Jiafa Chen,Yicheng Zhao,Yongdan Li
CO 2 formylation of amines provides a promising route to convert CO 2 into value-added chemicals. That process is usually performed through a thermo-catalytic approach with additional reducing agents, which increases the energy consumption and the complexity of the system. Herein, we report photocatalytic CO 2 formylation of benzylamine over Pt 1 In-ZnO x single-atom-alloy catalyst at room temperature in N , N -dimethylformamide (DMF) solvent. The anchoring of Pt single atoms onto In nanoparticles through Pt-In bonds accompanied with electron transfer from In to Pt improves the absorption capacity for visible light and the separation efficiency of photogenerated charge carriers. Furthermore, the adsorption and activation of CO 2 and benzylamine are promoted on the surface of Pt 1 In single-atom-alloy. After 6 h reaction under visible-light, the yield of N -benzylformamide reaches 48.6 mmol g −1 with a 95.3 % selectivity. A possible reaction mechanism is proposed based on a series of in situ characterizations and theoretical calculations. A decomposition-regeneration cycle of DMF is involved in the photocatalytic process, which extends the reaction region and thus facilitates the formylation of benzylamine. The photocatalytic system exhibits good cycling stability and universality. This work provides new insights for the rational design of single-atom-alloy catalyst and an efficient approach for the sustainable utilization of CO 2 .
研究领域:
化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2024
·
IF 18.5
Yumeng Li,Yingmin Jin,Xuebai Zhang,Mengyu Fu,Ruifan Lin,Guanshu Li,Yueping Xiong
The electrochemical CO 2 reduction reaction (ECO 2 RR) has emerged as a promising technology for achieving carbon neutralization. Even though considerable efforts are dedicated to gain deep insight into the understanding of ECO 2 RR on a mechanism level through density functional theory (DFT) studies, effects of solvent molecules and temperature have long been neglected by conventional DFT calculations as a consequence of limitations in current technologies and computational power of supercomputers. Under this context, the lack of comprehensive understanding over the energy changes in the reaction derived from the only concern on free energy changes between reaction intermediates have arouse an urgent call for exploring feasible calculation options toward generalized theoretical study. Here, a systematic mechanism study is provided toward ECO 2 RR via constrained ab initio molecular dynamics (cAIMD) simulations, in which the effects of solvent water molecules and temperature are taken into consideration to guide the synthesis of single-atom alloy (SAA) catalyst. Consequently, the resultant Pr 0.05 /InBi achieves a maximum Faradic efficiency (FE) of 96.4% and an energy efficacy (EE) of 59.41% for formate. This work offers a novel approach to the design and screening of SAA catalysts, presenting foreseeable future in accelerating the industrial application process of ECO 2 RR.
研究领域:
材料科学
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计算化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
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