INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
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IF 8.1
Xin Sun,Jun Wang,Jing Yu,Yifu Jing,Jingyuan Liu,Manish Singh,Peter D. Lund,Muhammad Imran Asghar
Atomic isolated and dispersed single atom catalyst is ideal for high-performance industrial catalyst. However, the contribution from small amounts of nanoclusters coexisting with single atoms to the catalytic reaction activity is often neglected. In this work, a MXene-supported uniformly dispersed Pt single atoms and nanoclusters (Pt 1 +Pt n /MXene) were obtained by self-assembly through an impregnation method. The catalyst exhibits high electrochemical performance in the hydrogen evolution reaction with an overpotential of only 61.3 mV and a Tafel slope of 32.5 mV dec −1 at a current density of 10 mA cm −2 in an acidic environment. The XAFS analysis and further DFT calculation indicate that the synergistic effect between single atoms and nanoclusters can facilitate adsorption of H* and promote the HER reaction. This work provides an efficient method for integrating multiple active sites in noble metal catalysts.
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
ACS Catalysis
·
2019
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IF 12.221
Yanfu Ma,Banlan Chi,Wei Liu,Lina Cao,Yue Lin,Xiaohui Zhang,Xuxu Ye,Shiqiang Wei,Junling Lu
Atomically dispersed metal atoms on supports, so-called single-atom catalysts (SACs), have recently attracted extensive attention in the catalysis field. It has been found that besides the primary metal atom, the proximial atoms also contribute to the catalytic activity significantly. Here, we show that tailoring of the local coordination environment of Pt1 single atoms on CeO2 using phosphorus gives rise to an activity enhancement up to a 10 times higher than Pt1/CeO2 SAC in hydrogenation of styrene, cyclohexene, phenylacetylene, and nitrobenzene. X-ray absorption, photoelectron, and infrared spectroscopies showed that the Pt1 single atoms modulated by phosphorus have a higher valence state. Infrared spectroscopy and temperature-programmed reduction further unveiled that significantly stronger adsorption of reactant and facilitated hydrogen spillover on phosphorus-doped CeO2 both play important roles for the dramatic activity enhancement. These findings point out an avenue to design an advanced SACs with high activity.
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
Small
·
2023
·Vol. 20
·期 20
·2307386
·
IF 13.3
Shiting Wu,Xiaohui Li,Jiaqi Liu,Hanfeng Wu,Hanshuai Xu,Wangfeng Bai,Liang Mao,Xiaowei Shi
Selective photocatalytic production of high-value acetaldehyde concurrently with H 2 from bioethanol is an appealing approach to meet the urgent environment and energy issues. However, the difficult ethanol dehydrogenation and insufficient active sites for proton reduction within the catalysts, and the long spatial distance between these two sites always restrict their catalytic activity. Here, guided by the strong metal-substrate interaction effect, an atomic-level catalyst design strategy to construct Pt-S 3 single atom on ZnIn 2 S 4 nanosheets (Pt SA -ZIS) is demonstrated. As active center with optimized H adsorption energy to facilitate H 2 evolution reaction, the unique Pt single atom also donates electrons to its neighboring S atoms with electron-enriched sites formed to activate the O─H bond in * CH 3 CHOH and promote the desorption of * CH 3 CHO. Thus, the synergy between Pt single atom and ZIS together will reduce the energy barrier for the ethanol oxidization to acetaldehyde, and also narrow the spatial distance for proton mass transfer. These features enable Pt SA -ZIS photocatalyst to produce acetaldehyde with a selectivity of ≈100%, which will spontaneously transform into 1,1-diethoxyethane via acetalization to avoid volatilization. Meanwhile, a remarkable H 2 evolution rate (184.4 µmol h −1 ) is achieved with a high apparent quantum efficiency of 10.50% at 400 nm.
研究领域:
材料科学
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催化化学
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能源转化
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
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IF 13.273
Yu Qiu,Shuangquan Liu,Cong Wei,Jianxiong Fan,Hu Yao,Lanxin Dai,Gongming Wang,Hong Li,Baolian Su,XiaoHui Guo
Single-atomic or cluster-based precious metals provide an effective pathway to minimize the cost of catalysts. However, its stability at large current density is still a major hurdle to satisfy practical requirements for electrocatalytic Hydrogen evolution reaction (HER). Herein, we successfully anchored Pt single atoms (Pt SAs) in the oxygen vacancies (O vac ) of Molybdenum dioxide (MoO 2 ) as advanced HER electrocatalyst. Experimental and theoretical calculations results reveal that the O vac can not only stabilize Pt SAs, but also modulate the electronic structure of the active site, enabling Pt SAs/MoO 2 to exhibit superior HER activity in a wide pH electrolyte at large current density. Especially, the 1.1 wt% Pt SAs/MoO 2 deliver ultralow overpotentials (9.3, 14, and 16 mV at 10 mA cm −2 ) and small Tafel slopes (28.78, 36.86, and 65.18 mV dec -1 ) in acidic, alkaline, and neutral electrolytes, respectively. Moreover, it displays significantly enhanced mass activity of up to 28, 32, and 56 times compared to the benchmark 20 wt% Pt/C catalyst, and outstanding long-term durability (~200 h) at large current density of −1000 mA cm −2 . The significantly improved HER performances are mainly ascribed to the synergistic catalytic effects of between Pt SAs and O vac in MoO 2 . These impressive findings can provide insights into the rational design of electrocatalysts that used for future clean energy utilization.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yushun Wang,Xinzheng Zhang,Yuquan Yang,Huichao Wang,Woon-Ming Lau,Chenjing Wang,Zhongheng Fu,Dawei Pang,Qian Wang,Jinlong Zheng
The single atom catalysts (SACs) show immense promise as catalytic materials. By doping the single atoms (SAs) of precious metals onto substrates, the atomic utilization of these metals can be maximized, thereby reducing catalyst costs. The electronic structure of precious metal SAs is significantly influenced by compositions of doped substrates. Therefore, optimizing the electronic structure through appropriate doping of substrates can further enhance catalytic activity. Here, Pt single atoms (Pt SAs) are doped onto transition metal sulfide substrate NiS 2 (Pt SAs-NiS 2 ) and phosphide substrate Ni 2 P (Pt SAs-Ni 2 P) to design and prepare catalysts. Compared to the Pt SAs-NiS 2 catalyst, the Pt SAs-Ni 2 P catalyst exhibits better hydrogen evolution catalytic performance and stability. Under 1 M KOH conditions, the hydrogen evolution mass activity current density of the Pt SAs-Ni 2 P catalyst reaches 0.225 A mg Pt –1 at 50 mV, which is 33 times higher than that of commercial Pt/C catalysts. It requires only 44.9 mV to achieve a current density of 10 mA cm −2 . In contrast, for the Pt SAs-NiS 2 catalyst, the hydrogen evolution mass activity current density is 0.178 A mg Pt –1 , requiring 77.8 mV to achieve a current density of 10 mA cm −2 . Theoretical calculations indicate that in Pt SAs-Ni 2 P, the interaction between Pt SAs and the Ni 2 P substrate causes the Pt d-band center to shift downward, enhancing the H 2 O desorption and providing optimal H binding sites. Additionally, the hollow octahedral morphology of Ni 2 P provides a larger surface area, exposing more reactive sites and improving reaction kinetics. This study presents an effective pathway for preparing high-performance hydrogen evolution electrocatalysts by selecting appropriate doped substrates to control the electronic structure of Pt SAs.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Youyu Pang,Rui Zhang,Linjia Li,Yanhong Lin,Ziheng Li,Tengfeng Xie
The anchoring sites of metal single atoms are closely related to photogenerated carrier dynamics and surface reactions. Achieving smooth photogenerated charge transfer through precise design of single-atom anchoring sites is an effective strategy to enhance the activity of photocatalytic hydrogen evolution. In this study, Pt single atoms were loaded onto ultra-thin carbon nitride with two-coordination nitrogen vacancies (V N2c -UCN-Pt) and ultra-thin carbon nitride with three-coordination nitrogen vacancies (V N3c -UCN-Pt). This paper investigated the photocatalytic hydrogen evolution performance and photogenerated carrier behavior of Pt single atoms at different anchoring sites. Surface photovoltage measurements indicated that V N2c -UCN-Pt exhibits a superior carrier separation efficiency compared to V N3c -UCN-Pt. More importantly, the surface photovoltage signal under the presence of H 2 O molecules revealed a significant decrease. Theoretical calculations suggest that V N2c -UCN-Pt exhibits superior capabilities in adsorbing and activating H 2 O molecules. Consequently, the photocatalytic hydrogen evolution efficiency of V N2c -UCN-Pt reaches 1774 µmol g −1 h −1 , which is 1.8 times that of V N3c -UCN-Pt with the same Pt loading. This work emphasized the structure–activity relationship between single-atom anchoring sites and photocatalytic activity, providing a new perspective for designing precisely dispersed single-atom sites to achieve efficient photocatalytic hydrogen evolution.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
·
IF 20.2
Shanpeng Li,Yuling Zhuo,Dong Liu,Hui Pan,Zhenbo Wang
Improving the Pt atoms utilization efficiency on self-supported electrodes is crucial for industrial seawater hydrogen production , but effective strategies are still lacking. Herein, we reported a novel strategy to anchor highly surface-exposed Pt single atoms on Ni 3 S 2 /Co 9 S 8 with abundant S vacancies (Pt–Ni 3 S 2 /Co 9 S 8 –Sv) as a self-supported electrode. Physical characterizations and theoretical calculations confirm that the strong Pt–S electron bridges with the coordinating role of surface S vacancies triggers the d -orbital electron rearrangements and regulates the local electron structures between the Co/Ni and Pt sites. Notably, the Pt–Ni 3 S 2 /Co 9 S 8 –Sv electrode displays an ultralow overpotential of 18 mV at 10 mA cm −2 in alkaline seawater . More importantly, our Pt–Ni 3 S 2 /Co 9 S 8 –Sv electrode assembled into an alkaline electrolysis cell can work continuously for 50 h under alkaline seawater @ 60 °C. This work provides a promising strategy for designing highly surface-exposed single-atomic catalyst for large-scale hydrogen evolution through seawater electrolysis.
研究领域:
材料科学
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催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Chang Lv,Tao Wang,Yeting Fang,Yulong Ying,Lvlv Ji,Lei Liu,Sheng Wang
Bubble-propelled catalytic micro-/nanomotors, known for their strong thrust, rapid speeds, and long lifespan independent of ionic strength, have attracted significant attention for applications in environmental remediation. While single-atom catalysts have demonstrated remarkable catalytic efficiency, their performance alone often lacks the necessary activity for efficient hydrogen peroxide (H2O2) decomposition, limiting their use in bubble-propelled systems. To address this, we present a novel approach for fabricating Pt-decorated titanium dioxide micro-bowls (PtSA&C-TiO2) featuring dual active sites with atomically dispersed Pt single atoms (SAs) and atomic clusters (Cs). This design capitalizes on the consistent metallic characteristics of Pt Cs, which significantly enhance the decomposition of H2O2 and propel the Janus micromotors to a speed of 113 ± 47 μm s−1 in aqueous solutions. Furthermore, these PtSA&C-TiO2 Janus micromotors exhibit excellent photocatalytic activity for pollutant degradation, which is enhanced by the synergistic effect of Pt SAs and Pt Cs. The study also discusses the factors influencing the self-assembly of Janus TiO2 micro-bowls, emphasizing the simplicity and controllability of the fabrication process, which enables large-scale production. This work not only demonstrates the potential of PtSA&C-TiO2 Janus micromotors for environmental applications, but also offers new insights into the design and application of single-atom-based micromotors.
研究领域:
环境科学
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材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Jiang Mo,Su Liu,Quan-Qing Xu,Xiang-Ying He,Wei-Hua Mu,Ming-Yu Teng,Wen-Fu Fu
In this work, Pt single atoms (SAs) were engineered on the surface of CdIn 2 S 4 (CIS) to trigger abundant generation and stable existence of sulfur vacancies (S v ). Through quasi in situ X-ray photoelectron spectroscopy (XPS) and work function analysis, the photogenerated electrons are first captured by Pt SAs and S v , and then transferred from Pt SAs to S v , ultimately increasing the electron density of S v . Meanwhile, S v have significant advantages in adsorbing CO 2 molecules. According to the number of transferred electrons, the optimized 0.8 %Pt/CIS has 76 times the photocatalytic performance of pristine CIS, and the selectivity of ethylene (C 2 H 4 ) is up to 99.3 %. The carbon–carbon coupling reaction between *CO and *CHO adsorbed on double sites of S v and In atoms is identified as the rate-determining step. Theoretical calculations suggest that the energy barrier required for coupling of intermediates *CO and *CHO is the lowest, conducive to the selective generation of C 2 H 4 .
研究领域:
材料科学
·
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Kuang Sheng,Guang Li,Min Liu,Lei Gan,Shiqi Huang,Jie Li
Optimizing the accessibility and chemical microenvironment of Pt single atoms (SAs) is essential for enhancing the efficiency of hydrogen evolution reaction (HER). Herein, we present a hierarchical catalyst (Pt 3 /WC/HS) featuring highly accessible Pt SAs moderately coordinated with WC nanoparticles and uniformly anchored on monodisperse porous carbon nanospheres. With a Pt content of 2.8 wt%, Pt 3 /WC/HS achieves an ultralow overpotential of 8 mV at 10 mA cm −2 , outperforming commercial 20 wt% Pt/C. Additionally, the catalyst exhibits outstanding HER activity in proton exchange membrane water electrolyzers (PEMWE), simulated seawater, and neutral media. Notably, in a coal-assisted hydrogen production system that decouples oxygen evolution reaction (OER) from HER, Pt 3 /WC/HS achieves 400 mA cm −2 at an applied potential of just 0.5 V. Spectroscopic characterizations and density functional theory (DFT) reveal that WC stabilizes the Pt SAs while retaining an active electronic configuration in the Pt 5 d z 2 orbital, shifting *H adsorption from thermodynamically unfavorable to spontaneous. Moreover, the interconnected porous framework of Pt 3 /WC/HS ensures high Pt site accessibility at the three-phase interface. This work demonstrates a versatile and high-performance HER catalyst suitable for diverse hydrogen evolution systems and offers a rational design strategy for single-atom catalysts.
研究领域:
材料科学
·
催化化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Chao Wang,Hu Zang,Changjiang Liu,Jiahao Wang,Long Kuai,Baoyou Geng
The hydrogen evolution reaction (HER) involves two-step elementary reactions, providing an opportunity to establish dual-site synergistic catalysts. This work demonstrates carbon-supported Pt single atoms and clusters (Pt1+Cs-NPC) as an efficient catalyst for acidic HER, which exhibits an ultralow Tafel slope of 12.5 mV/dec and an overpotential of 24 mV at 10 mA/cm2 with an ultralow platinum content of 3.8 wt %. The Pt mass activity and turnover frequency (TOF) are 10.2 times and 5.4 times that of commercial Pt/C, respectively. The density functional theory (DFT) study shows that the Pt cluster regulates the electronic state structure of the adjacent Pt single atom, so that the ΔGH* at the Pt1 site approaches 0. Moreover, the DFT study confirms that Pt clusters and neighboring Pt single atoms can synergistically catalyze the Tafel step and reduce the energy barrier in forming the H–H bond. At the same time, the platinum cluster reduces the energy barrier of the nearby platinum single-atom site to the Heyrovsky step and accelerates the reaction with hydrated hydrogen ions. Studies have shown that platinum clusters and platinum single-atom composite loading structures exhibit excellent activity for the Volmer–Tafel or Volmer–Heyrovsky reaction paths of HER reactions. This work provides a clear understanding of the synergistic effect of Pt1+Cs-NPC, which provides guidance for developing efficient HER catalysts.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
PubMed
高影响因子
CARBON
·
2022
·
IF 11.307
Chao Wang,Feiran Chen,Qinru Wang,Xiaofeng Yang,Hu Zang,Nan Yu,Baoyou Geng
Alkaline water electrolysis is a safe and efficient method for producing hydrogen that is favored by the industry. At present, single-atom catalysts have attracted extensive attention due to their extremely high atom utilization. However, studies on the single-atom site catalytic mechanism of the Volmer step, the rate-determining step of the cathodic HER reaction, are lacking. Here, we used ZIF-8 to obtain double-layer N-doped porous carbon nanocages, and successfully achieved the co-loading of Pt single atoms and their clusters (NPCN–Pt). The turnover frequency (TOF) and mass activity of NPCN–Pt are 5 and 7.2 times higher than those of commercial Pt/C, respectively, and the former exhibits significantly better stability than Pt/C. Theoretical calculations show that Pt clusters have a lower activation energy barrier for water molecules compared to Pt single atoms, which favors the Volmer step. The ΔG H* of Pt single-atom sites is smaller than that of Pt clusters, which is more conducive to the release of H 2 . The study shows that Pt clusters and single atoms can synergistically catalyze the HER reaction, providing new ideas for the development of efficient HER catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）