CHINESE JOURNAL OF CATALYSIS
·
2025
·
IF 17.7
Yangyang Li,Jingyi Yang,Botao Qiao,Tao Zhang
Supported metal catalysts are the backbone of heterogeneous catalysis, playing a crucial role in the modern chemical industry. Metal-support interactions (MSIs) are known important in determining the catalytic performance of supported metal catalysts. This is particularly true for single-atom catalysts (SACs) and pseudo-single-atom catalysts (pseudo-SACs), where all metal atoms are dispersed on, and interact directly with the support. Consequently, the MSI of SACs and pseudo-SACs are theoretically more sensitive to modulation compared to that of traditional nanoparticle catalysts. In this work, we experimentally demonstrated this hypothesis by an observed size-dependent MSI modulation. We fabricated CoFe 2 O 4 supported Pt pseudo-SACs and nanoparticle catalysts, followed by a straightforward water treatment process. It was found that the covalent strong metal-support interaction (CMSI) in pseudo-SACs can be weakened, leading to a significant activity improvement in methane combustion reaction. This finding aligns with our recent observation of CoFe 2 O 4 supported Pt SACs. By contrast, the MSI in Pt nanoparticle catalyst was barely affected by the water treatment, giving rise to almost unchanged catalytic performance. This work highlights the critical role of metal size in determining the MSI modulation, offering a novel strategy for tuning the catalytic performance of SACs and pseudo-SACs by fine-tuning their MSIs.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2025
·
IF 13.5
Yuchen Zhou,Huanmin Liu,Hongxing Li,Xinyu Song,Yonghua Tang,Peng Zhou
The intrinsic surface atomic configuration of photocatalyst without unstable or difficult-to-generate atomic vacancies often limits the formation of effective interaction between metal single atom (MSA) cocatalyst and photocatalyst, thus inhibiting the stability and performance improvement of single-atom photocatalysts. In this study, we present a convenient and cost-effective photochemical oxygen reduction reaction (ORR) mechanism to prepare thermodynamically stable noble metal single-atom cocatalysts on TiO 2 photocatalyst under mild condition (only consuming water and oxygen at 101,325 Pa and 25 °C). The first-principles simulation firstly theoretically reveals that the intrinsic surface configuration of TiO 2 can only produce unstable Pt―O 2 structure. However, ORR occurring on TiO 2 can not only provide one foreign oxygen to coordinate with Pt single atom (PtSA), but also induce one surface lattice oxygen to move toward PtSA, promoting the formation of one thermodynamically stable Pt―O 4 species, demonstrated by the experimental synthesis of PtSA on TiO 2 in oxygen atmosphere instead of inert atmosphere. The obtained stable PtSA-TiO 2 photocatalysts exhibit a photocatalytic rate of 320.4 mmol·g −1 ·h −1 for the coproduction of high-purity hydrogen and value-added acetaldehyde with a selectivity of 99.65%, three-fold higher than the activity of Pt nanoparticles-loaded TiO 2 . This strategy is further extended to other noble metals, such as Rh and Pd.
研究领域:
化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Zhou Yang,Meng Xiang,Yunfeng Zhu,Jia Hui,Yong Jiang,Shuang Dong,Chengbin Yu,Junfei Ou,Hengfei Qin
Pt/C is a practical electrocatalyst for oxygen reduction reaction (ORR) in metal-air batteries and fuel cells, however, also suffers the drawbacks of high cost and instability, which have propelled people to search for new substitutes, such as single-atom metal electrocatalysts. Herein, C 4 N was firstly synthesized from 2,3-diyldiamine phenazine via one-step hydrothermal method rather than the traditional way that two monomers react in organic solvent, and then loaded with single-atom metal (Pt or Ru) to form new electrocatalysts. The so-formed M@C 4 N (M = Pt or Ru) electrocatalysts show more excellent ORR performances with higher half-wave potential and better stability and methanol tolerance as compared with the commercial Pt/C. Specifically, the half-wave potential of 1%Pt@C 4 N and 0.5%Ru@C 4 N is 0.861 V and 0.828 V, respectively. Density functional theory calculations reveal that 1%Pt@C 4 N has stronger adsorption of reactant species and faster kinetics than 0.5%Ru@C 4 N in ORR pathway.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Shi Xiaowei,Dai Chao,Wang Xin,Hu Jiayue,Zhang Junying,Zheng Lingxia,Mao Liang,Zheng Huajun,Zhu Mingshan
Single-site cocatalysts engineered on supports offer a cost-efficient pathway to utilize precious metals, yet improving the performance further with minimal catalyst loading is still highly desirable. Here we have conducted a photochemical reaction to stabilize ultralow Pt co-catalysts (0.26 wt%) onto the basal plane of hexagonal ZnIn 2 S 4 nanosheets (Pt SS -ZIS) to form a Pt-S 3 protrusion tetrahedron coordination structure. Compared with the traditional defect-trapped Pt single-site counterparts, the protruding Pt single-sites on h -ZIS photocatalyst enhance the H 2 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g −1 h −1 under visible light irradiation. Importantly, through simple drop-casting, a thin Pt SS -ZIS film is prepared, and large amount of observable H 2 bubbles are generated, providing great potential for practical solar-light-driven H 2 production. The protruding single Pt atoms in Pt SS -ZIS could inhibit the recombination of electron-hole pairs and cause a tip effect to optimize the adsorption/desorption behavior of H through effective proton mass transfer, which synergistically promote reaction thermodynamics and kinetics.
研究领域:
材料科学
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能源化学
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环境科学
✓ 已验证
DOI
高影响因子
ACS Applied Nano Materials
·
2024
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IF 5.3
Xihui Lu,Jinshan Wei,Hexing Lin,Yi Li,Ya-yun Li
Electrocatalytic reduction of nitrate (NO3RR) to ammonia offers a promising approach for mitigating the environmental impact of NO3–, while simultaneously enabling the synthesis of NH3 under ambient conditions. Recently, single-atom catalysts (SACs) have been proven to have attractive activity on NO3RR, and better catalysts with enhanced activity and stability are still in demand. Here, we report the efficient boosting of NH3 production via the NO3RR using boron-doped Fe SAC (Fe-BCN). Fe-BCN is a normal 12-hedral nanoparticle with a size of 500 nm. The NH3 Faradaic efficiency of Fe-BCN reached 97.48%, with a high ammonia production rate of 2.17 mg cm–2 h–1, in an alkaline electrolyte environment at an electrode potential of −0.3 V vs reversible hydrogen electrode. Density functional theory calculations revealed the strategy of introduced B regulating the intermediate adsorption on Fe-BCN, which enhanced the NO3RR activity. Furthermore, leveraging the high NO3RR activity of Fe-BCN, a nitrate-zinc battery with a power density of 0.90 mW cm–2 was constructed by using Fe-BCN as the cathode and zinc as the anode, respectively. This research demonstrates the broad prospects of Fe-BCN in the NO3RR and provides insights for high-performance Fe SAC electrode materials.
研究领域:
催化化学
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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
ChemCatChem
·
2021
·Vol. 13
·期 7
·1834-1846
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IF 5.686
Ruihuan Jiang,Shaomian Liu,Liang Li,Yongjun Ji,Huifang Li,Xiangfeng Guo,Lihua Jia,Ziyi Zhong,Fabing Su
Graphical Single Ir atoms : In the CO+NO reaction, the catalyst with single-sited Ir atoms (0.28 wt %) anchored on a mesoporous WO 3 (Ir 1 /mesoporous-WO 3 ) showed much higher NO conversion and N 2 selectivity under oxygen-rich conditions than the catalysts supported with Ir nanoparticles on the same catalyst support (Ir NPs/mesoporous-WO 3 ) and on a non-mesoporous WO 3 (Ir/non-mesoporous-WO 3 ). Under oxygen-rich conditions, achieving a selective and efficient reduction of NO by CO is always challenging. Here, we report the synthesis of the catalyst consisting of single Ir atoms anchored on mesoporous WO 3 (denoted as Ir 1 /m-WO 3 ) using a facile template method followed by wet impregnation. X-ray diffraction and transmission electron microscope studies indicated that the Ir atoms were distributed uniformly on the internal surface of m-WO 3 . When tested for the reduction of NO by CO, the Ir 1 /m-WO 3 catalyst with a low Ir loading of 0.28 wt % exhibited excellent catalytic performance in the presence of 2 vol % O 2 (volume ratio of CO to O 2 being 1 : 10), achieving a NO conversion of 73 % and N 2 selectivity of 100 % at 350 °C. In particular, its turnover frequency (TOF) value reached 0.30 s −1 at 200 °C, which is six times higher than that of the catalyst with Ir nanoparticles supported on mesoporous WO 3 (0.05 s −1 ). The superior catalytic performance of Ir 1 /m-WO 3 is attributed to the formation of the isolated Ir atoms and the more newly generated Ir-WO 3 interfaces that can promote the adsorption and activation of NO, and the presence of accessible mesopores in m-WO 3 that facilitates the mass transfer of NO and CO. This study brings a new fundamental understanding of active sites in Ir-based catalysts for the CO+NO reaction and provides a new way to the design and synthesis of single-atom catalysts, especially precious metal catalysts for emissions control.
研究领域:
催化化学
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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
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Cailing Wu,Mingming Sun,Xinyang Gao,Qifei Huang,Zhaojun Min,Yanxing Zhang,Jianji Wang
Single atom catalysts (SACs) supported on metal oxide are usually prepared at high temperature, high pressure, and complex process. Herein, a new strategy is developed to prepare SACs anchored on vacancy-rich TiO 2 using Ti 2 O 3 as the support precursor under mild conditions, where Ti 3+ on Ti 2 O 3 surface acts as “traps” to capture and then reduce metal ions through electron transfer without using reducing agents. This approach is universally applicable for different single metal atoms supported on diverse phases of TiO 2 (anatase, rutile, metastable and mixed counterpart). The as-obtained Pt 1 /TiO 2 with controllable Pt loading and multiple oxygen vacancies (Ov) exhibits excellent activity in photocatalytic H 2 evolution. At optimal conditions, the H 2 evolution rate is up to 95,180 μmol g −1 h −1 , which is the highest for TiO 2 supported SACs reported.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Xiaoqian Hao,Shengjun Xu,Yan Huang,Shuanglong Ma,Boqiang Gao,Jia Song,Jingzhen Wang,Sihui Zhan
Molybdenum disulfide serves as an ideal support for single atom catalysts (SACs), offering not only coordination elements but also abundant active sites, such as surface defects and vacancies. Herein, a novel Co-SAC (MoSO-Co-C) containing a four-coordinated configuration (Mo-Co-C 3 ) is designed and synthesized, in which the carbon intercalation is utilized to regulate sulfur vacancies for anchoring the Co atom. The introduction of Co atoms and C intercalation significantly enhances the E ads between catalyst and peroxymonosulfate (PMS), favoring the formation of metastable intermediates. The k obs of sulfamethoxazole (SMX) removal for MoSO-Co-C is 9.2 times and 1.8 times higher than those of catalysts without Co or C intercalation. SMX is removed mainly by electron transfer pathway, wherein SMX and PMS act on the same Co site of MoSO-Co-C, and electrons are transferred from SMX to MoSO-Co-C and eventually to PMS. The MoSO-Co-C demonstrated excellent SMX degradation in the diverse water matrices, and the removal efficiency of SMX maintained above 95 % after 72 h of continuous degradation. This study provides new insights into the design of transition metal-based SAC and in-depth understanding of PMS activation mechanism.
研究领域:
环境科学
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催化
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水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Cenyu Yang,Chen Hu,Xiaoyu Wu,Yao Pang,Xiaofang Liu,Jianglan Shui
Metallic single-atom catalysts (SACs) have demonstrated high activity and potential in enhancing the hydrogen storage properties of MgH 2 . However, previous reports primarily focus on supported SACs, which often suffer from insufficient contact between single-atom active sites and hydrogen storage materials. In this study, the precursor Mo(CO) 6 is uniformly dispersed on the surface of MgH 2 via impregnation adsorption, leading to the formation of alloy-type Mo single atoms after hydrogenation/dehydrogenation activation. This alloy structure enables zero-distance contact between catalytic sites and the hydrogen storage material, facilitating electron exchange and hydrogen transfer between the Mo sites and MgH 2 . The MgH 2 loaded with Mo single atoms (Mo 1 -MgH 2 ) exhibits excellent hydrogen absorption and desorption properties, with the initial hydrogen release temperature lowered from 323 to 218 °C. At 250 °C, Mo 1 -MgH 2 absorbs over 6.77 wt% of hydrogen within 1 min and releases over 5.85 wt% within 4 h. During 10 cycles of hydrogenation and dehydrogenation reactions, Mo 1 -MgH 2 maintains nearly 100% capacity and shows stable kinetics. This work provides new insights into the design and fabrication of catalysts for hydrogen storage materials.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2020
·Vol. 11
·期 1
·1-9
·
IF 12.121
Liu Kaipeng,Zhao Xintian,Ren Guoqing,Yang Tao,Ren Yujing,Lee Adam Fraser,Su Yang,Pan Xiaoli,Zhang Jingcai,Chen Zhiqiang,Yang Jingyi,Liu Xiaoyan,Zhou Tong,Xi Wei,Luo Jun,Zeng Chaobin,Matsumoto Hiroaki,Liu Wei,Jiang Qike,Wilson Karen,Wang Aiqin,Qiao Botao,Li Weizhen,Zhang Tao
Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions. However, producing thermally stable SACs, especially in a simple and scalable way, remains a formidable challenge. Here, we report the synthesis of Ru SACs from commercial RuO 2 powders by physical mixing of sub-micron RuO 2 aggregates with a MgAl 1.2 Fe 0.8 O 4 spinel. Atomically dispersed Ru is confirmed by aberration-corrected scanning transmission electron microscopy and X-ray absorption spectroscopy. Detailed studies reveal that the dispersion process does not arise from a gas atom trapping mechanism, but rather from anti-Ostwald ripening promoted by a strong covalent metal-support interaction. This synthetic strategy is simple and amenable to the large-scale manufacture of thermally stable SACs for industrial applications.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
DOI
PubMed
高影响因子
The Innovation
·
2022
·Vol. 3
·期 4
·100268-100268
·
IF 0
Zichuang Li,Ruguang Ma,Qiangjian Ju,Qian Liu,Lijia Liu,Yufang Zhu,Minghui Yang,Jiacheng Wang
Single-site metal atoms (SMAs) on supports are attracting extensive interest as new catalytic systems because of maximized atom utilization and superior performance. However, rational design of configuration-optimized SMAs with high activity from the perspectives of fundamental electron spin is highly challenging. Herein, N-coordinated Fe single atoms are successfully distributed over axial carbon micropores to form dangling-FeN 4 centers (d-FeN 4 ). This unique d-FeN 4 demonstrates much higher intrinsic activity toward oxygen reduction reaction (ORR) in HClO 4 than FeN 4 without micropore underneath and commercial Pt/C. Both theoretical calculation and electronic structure characterization imply that d-FeN 4 endows central Fe with medium spin (t 2g 4 e g 1 ), which provides a spin channel for electron transition compared with FeN 4 with low spin. This leads to the facile formation of the singlet state of oxygen-containing species from triplet oxygen during the ORR, thus showing faster kinetics than FeN 4 . This work provides an in-depth understanding of spin tuning on SMAs for advanced energy catalysis.
研究领域:
催化化学
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材料科学
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理论计算
✓ 已验证
DOI
PubMed
Small
·
2021
·Vol. 17
·期 52
·2105643
·
IF 13.281
Bo Liu,Linjuan Zhang,Yuanyuan Luo,Lei Gao,Guotao Duan
The supported metal catalysts on scaffolds usually reveal multiple active sites, resulting in the occurrence of side reaction and being detrimental to the achievement of highly consistent catalysis. Single atom catalysts (SACs), possessed with highly consistent single active sites, have great potentials for overcoming such issues. Herein, the authors used SACs to modulate kinetic process of gas sensitive reaction. The supported Pd SACs, established by a metal organic frameworks-templated approach, promoted greatly the detection capacity to hydrogen sulfide (H 2 S) gas with a very high sensitivity and selectivity. Density functional theory calculations show that the supported Pd SACs not only increased the number of electrons transferring from H 2 S molecules to Pd SACs, but strengthened surface affinity to H 2 S. Moreover, the H S bonds of H 2 S molecules absorbed on Pd atomic sites are more likely to be dehydrogenated directly into sulfur species. Significantly, quasi in situ XPS analysis confirmed the presence of sulfur species during H 2 S detection process, which may be a major cause for such detection signal. Based on these results, a suitable sensing principle for H 2 S gas driven by Pd SACs was put forward. This work will enrich catalytic electronics in chemiresistive gas sensing.
研究领域:
材料科学
·
催化化学
·
气体传感
✓ 已验证
DOI
PubMed
高影响因子
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