FUEL
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2025
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IF 7.5
Lei Sun,Mingjie Liu,Zepeng Hou,Xiaofeng Gao,Ziyu Song,Houhong Song,Zixuan Ma,Xinru Wu,Chuanmin Ding,Junwen Wang,Yuanyuan Meng,Siyu Yao
Hydrogen has been hailed as the quintessential energy resource for the future advancement of a carbon–neutral society. However, the storage and transportation of hydrogen present significant challenges due to its low density and high risk of explosion. The catalytic hydrolysis of sodium borohydride under mild conditions offers a viable solution to the aforementioned obstacles. Thus, the development and design of efficient, cost-effective and stable catalysts have attracted increasing attention to overcome the limitations and facilitate the practical application of this technology. In this study, an effective approach developed for fabricating a series of matrix catalysts that exhibit single-atom platinum (Pt) and cobalt (Co) nanocluster interface sites through a sequential immersion-reduction procedure. The findings revealed that the content of Pt and immersion sequence significantly influence catalyst performance. With its optimal structure, the 0.7 % Pt-4 % Co/C catalyst, prepared with a sequential immersion of Co followed by Pt, demonstrated a superior turnover frequency (TOF, based on the Pt content) of 1351 mol H2 mol Pt −1 min −1 at 298 K, which is 135 times higher than that of the Pt/C catalyst. Density functional theory (DFT) calculations and isotope labeling experiments underscore the significance of water activation in the hydrolysis reaction of NaBH 4 , which is augmented through the incorporation of single-atom Pt and Co nanocluster. These findings provide novel perspectives on the design of catalysts for hydrogen evolution from NaBH 4 and open up new possibilities for their practical application in chemical hydrogen storage.
研究领域:
化学
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材料科学
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能源研究
✓ 已验证
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
Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
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IF 14.919
Shi Yi,Ma Zhi-Rui,Xiao Yi-Ying,Yin Yun-Chao,Huang Wen-Mao,Huang Zhi-Chao,Zheng Yun-Zhe,Mu Fang-Ya,Huang Rong,Shi Guo-Yue,Sun Yi-Yang,Xia Xing-Hua,Chen Wei
Tuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.
研究领域:
催化
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电化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Wenliang Wang,JiangYuan Qiu,Tao Yu,Shuming Zhang,Xingwang Niu,Rui Guo,Jinsheng Li,Xuanwen Liu
Neutral aqueous Zn-air batteries have emerged as a compelling alternative to conventional alkaline systems, retaining inherent corrosion resistance and long-term stability while preserving high theoretical energy density. However, their practical application is hindered by sluggish oxygen evolution/reduction reaction (OER/ORR) kinetics and low ionic conductivity in neutral electrolytes, which result in a substantial charge-discharge voltage gap exceeding 600 mV. To address these challenges, this study employs a facile acetonitrile-mediated photocatalytic radical strategy to synthesize TiO₂-supported platinum single-atom (Pt₁/TiO₂) photoanodes under ambient conditions. Compared to pristine TiO₂, the Pt₁/TiO₂ photoanode demonstrates a 73 % enhancement in photocurrent density (reaching 2.11 mA cm⁻²) in neutral electrolytes and retains 92 % of its initial activity after 10 h of continuous illumination. Density functional theory calculations reveal that Pt single atoms not only serve as active sites but also modulate the electronic structure of adjacent Ti atoms. This strengthened Ti 3d z ²−O 2p z ² orbital hybridization optimizes *O intermediate adsorption, thereby reducing the energy barrier (η) of the OER rate-determining step to 1.81 eV. By integrating the Pt₁/TiO₂ photoanode with a CuO photocathode, we construct a dual-electrode photo-assisted neutral Zn-air battery (DEPZAB) that achieves a low charging voltage of 0.81 V at 0.1 mA cm⁻² and a record-breaking round-trip efficiency of approximately 145 %, outperforming traditional alkaline systems in cycling stability. These findings underscore the transformative potential of single-atom engineering in advancing sustainable energy storage technologies.
研究领域:
材料科学
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电化学
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能源存储
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光催化
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纳米材料
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可持续能源技术
✓ 已验证
产品关联
DOI
高影响因子
Theranostics
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2022
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IF 11.6
Qiqi Xu,Yuetong Zhang,Zulu Yang,Guohui Jiang,Mingzhu Lv,Huan Wang,Chenghui Liu,Jiani Xie,Chengyan Wang,Kun Guo,Zhanjun Gu,Yuan Yong
Nanozyme-based tumor collaborative catalytic therapy has attracted a great deal of attention in recent years. However, their cooperative outcome remains a great challenge due to the unique characteristics of tumor microenvironment (TME), such as insufficient endogenous hydrogen peroxide (H 2 O 2 ) level, hypoxia, and overexpressed intracellular glutathione (GSH). Methods: Herein, a TME-activated atomic-level engineered PtN 4 C single-atom nanozyme (PtN 4 C-SAzyme) is fabricated to induce the “butterfly effect” of reactive oxygen species (ROS) through facilitating intracellular H 2 O 2 cycle accumulation and GSH deprivation as well as X-ray deposition for ROS-involving CDT and O 2 -dependent chemoradiotherapy. Results: In the paradigm, the SAzyme could boost substantial ∙OH generation by their admirable peroxidase-like activity as well as X-ray deposition capacity. Simultaneously, O 2 self-sufficiency, GSH elimination and elevated Pt 2+ release can be achieved through the self-cyclic valence alteration of Pt (IV) and Pt (II) for alleviating tumor hypoxia, overwhelming the anti-oxidation defense effect and overcoming drug-resistance. More importantly, the PtN 4 C-SAzyme could also convert O 2 ·- into H 2 O 2 by their superior superoxide dismutase-like activity and achieve the sustainable replenishment of endogenous H 2 O 2 , and H 2 O 2 can further react with the PtN 4 C-SAzyme for realizing the cyclic accumulation of ∙OH and O 2 at tumor site, thereby generating a “key” to unlock the multi enzymes-like properties of SAzymes for tumor-specific self-reinforcing CDT and chemoradiotherapy. Conclusions: This work not only provides a promising TME-activated SAzyme-based paradigm with H 2 O 2 self-supplement and O 2 -evolving capacity for intensive CDT and chemoradiotherapy but also opens new horizons for the construction and tumor catalytic therapy of other SAzymes.
研究领域:
癌症治疗
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材料科学
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生物化学
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纳米医学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
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2022
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IF 18.027
Bowen Liu,Ruohan Feng,Michael Busch,Sihong Wang,Haofei Wu,Pan Liu,Jiajun Gu,Ashkan Bahadoran,Daiju Matsumura,Takuya Tsuji,Di Zhang,Fang Song,Qinglei Liu
Pt single-atom materials possess an ideal atom economy but suffer from limited intrinsic activity and side reaction of producing H2O2 in catalyzing the oxygen reduction reaction (ORR); platinum alloys have higher intrinsic activity but weak stability. Here, we demonstrate that anchoring platinum alloys on single-atom Pt-decorated carbon (Pt-SAC) surmounts their inherent deficiencies, thereby enabling a complete four-electron ORR pathway catalysis with high efficiency and durability. Pt3Co@Pt-SAC demonstrates an exceptional mass and specific activities 1 order of magnitude higher than those of commercial Pt/C. They are durable throughout 50000 cycles, showing only a 10 mV decay in half-wave potential. An in situ Raman analysis and theoretical calculations reveal that Pt3Co core nanocrystals modulate electron structures of the adjacent Pt single atoms to facilitate the intermediate absorption for fast kinetics. The superior durability is attributed to the shielding effect of the Pt-SAC coating, which significantly mitigates the dissolution of Pt3Co cores. The hybridizing strategy might promote the development of highly active and durable ORR catalysts.
研究领域:
材料科学
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电化学
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催化
✓ 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）