CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Jiaxin Huang,Chongshuai Gao,Shijun Liu,Xiaorui Du,Wenguang Zhou,Chenguang Wang
Alloying Cu-based catalysts by doping other metals at single atom level is an effective way to improve their hydrogenation performance of biomass-derived molecules. However, the application of Cu-based single atom alloy catalyst in the catalytic hydrogen transfer reaction system remains to be unrevealed. Here, we develop Al 2 O 3 supported CuPd alloy catalysts, among which the single atom alloy catalyst with Pd dispersed in single atomic level on the surface was successfully obtained by controlling the metal amount, such as Cu 8 Pd 1 /Al 2 O 3 with the Cu/Pd Molar ratio of 8: 1. The catalytic performance for furfural hydrodeoxygenation to 2-methylfuran of the CuPd/Al 2 O 3 catalysts, using isopropanol as a hydrogen donor, shows a volcano-type relationship to the Cu/Pd ratio. The highest 2-methylfuran yield (81% at 220 °C) was achieved on the single atom alloy catalyst Cu 8 Pd 1 /Al 2 O 3 . The underlying reaction mechanism of furfural hydrodeoxidation on Cu 8 Pd 1 /Al 2 O 3 was revealed by a series of isotopic labeling experiments, that the furfural was firstly hydrogenated to be furfuralcohol by a metal site-mediated catalytic transfer hydrogenation pathway, and then the furfuralcohol was converted to be 2-methylfuran by a Lewis acid-mediated furan ring activation route. The weak Lewis acid site that formed by single atom Pd alloyed with CuO matrix on Cu 8 Pd 1 /Al 2 O 3 was proposed as the active site for the highly selective generation of 2-methylfuran.
研究领域:
催化化学
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材料科学
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生物质转化
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产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-12
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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
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产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-9
·
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
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DOI
PubMed
高影响因子
International Journal of Electrochemical Science
·
2023
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IF 1.5
Jun Li,Xiaosi Liang,Chenyang Zhao
Pd is a promising anodic catalyst for direct formic acid fuel cells, while its performance on formic acid electrooxidation is still suffered from for low catalytic efficiency and durability. In this work, an electrochemical self-catalyzed method was employed to deposit Au single-atoms onto Pd nanocrystals with tuneable compositions . Spherical-corrected Scanning transmission microscope and electrochemical characteristics demonstrated that the Au atoms were atomic-dispersive on Pd nanocrystals, forming Au-Pd single-atom alloy. Systematic studies showed that the activity of Pd x @Au y /C SAA is related to the density of the Au single-atoms on Pd surface. When an optimized balance between active-site exposure and intrinsic activity is achieved, the Pd 50 @Au 1 /C SAA showed superb formic acid electrooxidation activity of 4.98 A mg −1 M and unusual high anti-poisoning ability which is distinctly different from most of the Pd based catalysts. The boosted electrochemical performances of Pd x @Au y /C SAA can be attributed to the unique geometric effect that facilitates the direct reaction route and favourable electronic effect that weakens the CO adsorption to Pd sites.
研究领域:
材料科学
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电化学
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产品关联
DOI
高影响因子
Nano-Micro Letters
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2025
·Vol. 17
·期 1
·1-14
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IF 36.3
Liao Yujia,Chen Wen,Ding Yutian,Xie Lei,Yang Qi,Wu Qilong,Liu Xianglong,Zhu Jinliang,Feng Renfei,Fu Xian-Zhu,Luo Shuiping,Luo Jing-Li
A unique catalyst surface where ultrathin Pt edges are modified by the isolated Pd atoms and BiO x adatoms is rational designed and achieved.
The Pd 1 /Pt-BiO x electrocatalyst exhibits an ultrahigh mass activity of 16.01 A mg −1 Pt+Pd toward ethanol oxidation and enables a direct ethanol fuel cell of peak power density of 56.7 mW cm −2 .
The surrounding BiO x adatoms are critical for mitigating CO-poisoning on Pt surface, and the Pd 1 /Pt single-atom alloy further facilitates the electrooxidation of CH 3 CH 2 OH.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2025
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IF 13.1
Yuanjing Zhang,Guanyi Zhang,Quandong Hou,Shiquan Zhao,Si Wang,Enze Xu,Lei Wang,Xin Zhang,Feng Li,Yusen Yang,Min Wei
Aqueous-phase tandem reactions, as a fundamental aspect of green chemistry, hold a crucial position in the contemporary synthesis of fine chemicals, wherein the advancement of high-performance heterogeneous catalysts remains a formidable challenge. Herein, we report a Pt1Con single-atom alloy (SAA) catalyst in which Pt single atoms are immobilized onto the surface of Co nanoparticles through Pt–Co coordination. The Pt1Con SAA catalyst exhibits a high chemoselectivity for the aqueous-phase hydrogenation–rearrangement reaction of furfural (FAL) to cyclopentanol (CPL) (yield: >93%, considering the carbon loss), with a TOF value of 2257 h–1 (based on Pt). A joint investigation based on reaction dynamics, isotope-label tracing experiments, EPR, and in situ FT-IR verifies a five-step consecutive tandem reaction pathway for the formation of CPL. Notably, during the reaction, the rapid exchange of hydrogen atoms would occur between activated hydrogen species and the water solvent. Furthermore, the water molecule does not serve as a H-donor but is involved in the rearrangement reaction in the side chain of the furan ring. Kinetic studies combined with DFT calculations substantiate that the Pt–Co interface sites effectively lower the energy barrier of the cyclopentanone (CPO) hydrogenation step via facilitating activation adsorption of the carbonyl group, accounting for the largely enhanced catalytic behavior. This study sheds light on the advancement of a highly efficient and stable heterogeneous catalyst for a biomass upgrading reaction in the aqueous phase.
研究领域:
绿色化学
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催化剂开发
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生物质转化
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产品关联
DOI
高影响因子
Nano Energy
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2025
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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
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产品关联
DOI
高影响因子
ChemCatChem
·
2023
·Vol. 15
·期 6
·e202300217
·
IF 4.5
Shanshan Chai,Denglei Gao,Jing Xia,Yanpeng Yang,Xi Wang
Graphical Alloy catalyst for acetylene hydrogenation: A palladium-silver dilute alloy catalyst (Pd x Ag/Al 2 O 3 ) was fabricated and showed an outstanding performance for acetylene hydrogenation, which contains the Pd 1 Ag single-atom-alloy (SAA) and Pd 2 Ag dimer-alloys (DA) species. Selective hydrogenation of acetylene (C 2 H 2 ) to ethylene (C 2 H 4 ) has been recognized as an important strategic reaction for the removal of trace acetylene from ethylene. Palladium-based alloys are one of the most commonly used catalysts for this reaction but bear a high price and unsatisfactory catalytic performance. Here, we develop a feasible strategy toward the synthesis of a palladium-silver dilute alloy catalyst (Pd x Ag/Al 2 O 3 ), which contains the Pd 1 Ag single-atom-alloy (SAA) and Pd 2 Ag dimer-alloy (DA) species. This catalyst exhibits a high ethylene (C 2 = ) yield of 90.1 % even after 100 hours at 60 °C, which is 11.9 times higher than that of the PdAg/Al 2 O 3 alloy catalyst. Based on in-situ spectroscopic investigations and theoretical calculations, both Pd 1 Ag SAA and Pd 2 Ag DA species in Pd x Ag/Al 2 O 3 are easier to desorb C 2 H 4 compared with PdAg/Al 2 O 3 , and they experience the possible hydrogenation paths with the low energy barriers to yield C 2 = . Furthermore, Pd x Ag/Al 2 O 3 is beneficial to restraining coking due to the endothermic C−H bond cleavage. Thus, these combined merits contribute to the superior catalytic performance for Pd x Ag/Al 2 O 3 .
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
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2022
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IF 10.383
Jun Li,Xiaosi Liang,Liying Cai,Shuke Huang,Chenyang Zhao
Single atom alloys (SAA) have recently drawn increased attention due to their unique structure, high atomic utilization, and fascinating catalytic performance. However, their controllable synthesis still presents a challenge. This study proposes an electrochemical self-catalysis (ESC) strategy to synthesize Pd@Pt/C SAA catalysts, that is, depositing Pt atoms on Pd nanocrystals through in situ decomposition of sodium formate. The relationship between composition and structure of Pd@Pt/C is distinguished through a combination of electrochemical analysis, sphere-corrected scanning transmission electron microscopy, and X-ray adsorption spectra. That relationship evolved from SAA to a sea-island structure and even a core–shell structure with composition-controllable atomic ratios, highlighting the great diversity and convenience of this method in nanostructure construction. The Pd@Pt/C SAA catalyst showed excellent catalytic activity to formic acid oxidation with a peak current density of 5.2 A/mgmetal, which is about 18.6 times that of the commercial Pd/C. density functional theory calculations revealed that the enhanced activity was due to the “passivation” of Pd sites near the Pt single atoms, which attenuated the adsorption of CO. Based on electrochemical principles, this ESC strategy was also expanded to prepare a series of Pd-based SAA, including Pd–Au, Pd–Ir, and Pd–Bi.
研究领域:
材料科学
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电化学
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催化化学
✓ 已验证
DOI
PubMed
高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2025
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IF 8.5
Sun Siyu,Zhang Feifei,Liu Wanlin,Zhang Rui,Yin Pengfei,Yang Jing,Dong Cunku,Nie Xinming,Liu Hui,Du Xiwen
The development of highly active and cost-effective catalysts for the full pH range of the hydrogen evolution reaction (HER) to meet the industrial application demands is an urgent challenge. In this work, the performance and structure–activity relationships of CuIr alloys prepared by the pulsed laser ablation in liquid technique as full pH range HER catalysts were investigated. Results indicated that Ir is doped into the Cu matrix as single atoms in CuIr-0.1, and CuIr-0.1 single-atom alloys (SAAs) exhibit superior HER performance and stability across the full pH range, with overpotentials of 135, 203, and 172 mV at the current density of 10 mA/cm 2 in acidic, neutral, and alkaline electrolytes, respectively. The enhanced performance of CuIr-0.1 SAAs can be attributed to the abundant active sites and accelerated reaction kinetics brought about by the electronic effects. This work successfully alloyed two immiscible metals to improve the catalytic performance, providing an avenue for the development of highly efficient and versatile HER catalysts for industrial applications.
研究领域:
材料科学
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电化学
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能源催化
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2022
·Vol. 10
·期 46
·24701-24707
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IF 14.511
Yu-Chuan Jiang,Yu Ding,Fu-Min Li,Shi-Bin Yin,Dong-Sheng Li,Xi-Fei Li,Yu Chen
The intrinsically sluggish kinetics of Pt towards the formate oxidation reaction (FOR) severely impedes its application in direct formate fuel cells (DFFCs). This study reports the synthesis of ultrafine Pd@PdPt nanowires (NWs) with a Pd–Pt single-atom alloy shell via an atomic galvanic displacement reaction. Pd@PdPt0.024 NWs with optimized composition exhibit a remarkable promoted specific activity of 98.2 A m−2 at 0.59 V towards the FOR, which is a 6.5- and 117.7-fold activity enhancement compared to original Pd NWs and commercial Pt catalysts. Density functional theory (DFT) calculations reveal that the electronic interaction between Pd and Pt as well as the modified Pt coordination environment endow the atomically dispersed Pt active site with an altered d-band structure and unique adsorption properties with a broken scaling relationship. The development of Pd@PdPt0.024 NWs will stimulate deeper insight into the FOR mechanism on Pt and hold promise for practical applications in DFFCs.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-11
·
IF 14.7
Xue Jing,Dong Xue,Liu Chunxiao,Li Jiawei,Dai Yizhou,Xue Weiqing,Luo Laihao,Ji Yuan,Zhang Xiao,Li Xu,Jiang Qiu,Zheng Tingting,Xiao Jianping,Xia Chuan
Using renewable electricity to convert CO 2 into CO offers a sustainable route to produce a versatile intermediate to synthesize various chemicals and fuels. For economic CO 2 -to-CO conversion at scale, however, there exists a trade-off between selectivity and activity, necessitating the delicate design of efficient catalysts to hit the sweet spot. We demonstrate here that copper co-alloyed with isolated antimony and palladium atoms can efficiently activate and convert CO 2 molecules into CO. This trimetallic single-atom alloy catalyst (Cu 92 Sb 5 Pd 3 ) achieves an outstanding CO selectivity of 100% (±1.5%) at −402 mA cm −2 and a high activity up to −1 A cm −2 in a neutral electrolyte, surpassing numerous state-of-the-art noble metal catalysts. Moreover, it exhibits long-term stability over 528 h at −100 mA cm −2 with an FE CO above 95%. Operando spectroscopy and theoretical simulation provide explicit evidence for the charge redistribution between Sb/Pd additions and Cu base, demonstrating that Sb and Pd single atoms synergistically shift the electronic structure of Cu for CO production and suppress hydrogen evolution. Additionally, the collaborative interactions enhance the overall stability of the catalyst. These results showcase that Sb/Pd-doped Cu can steadily carry out efficient CO 2 electrolysis under mild conditions, challenging the monopoly of noble metals in large-scale CO 2 -to-CO conversion.
研究领域:
材料科学
·
化学工程
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电化学
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可持续能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）