4.8 Article

Hexagonal PtBi Intermetallic Inlaid with Sub-Monolayer Pb Oxyhydroxide Boosts Methanol Oxidation


Volume 18, Issue 14, Pages -


DOI: 10.1002/smll.202107803


electrocatalysis; intermetallic; methanol oxidation; Pb oxyhydroxide


  1. National Natural Science Foundation of China (NSFC) [52101259, 21771156]
  2. National Key R&D Program of China [2021YFA1501101]
  3. Guangdong Science and Technology Department [2016ZT06C279]
  4. Shenzhen Science and Technology Innovation Committee [KQTD2016053019134356]
  5. National Natural Science Foundation of China/RGC Joint Research Scheme [N_PolyU502/21]
  6. Hong Kong Polytechnic University [1-ZE2V]

Ask authors/readers for more resources

The surface inlay of sub-monolayer Pb oxyhydroxide onto hexagonal PtBi intermetallic nanoplates can enhance the activity of methanol oxidation reaction, providing an effective nanoengineering strategy.
Engineering multicomponent nanocatalysts is effective to improve electrocatalysis in many applications, yet it remains a challenge in constructing well-defined multimetallic active sites at the atomic level. Herein, the surface inlay of sub-monolayer Pb oxyhydroxide onto hexagonal PtBi intermetallic nanoplates with intrinsically isolated Pt atoms to boost the methanol oxidation reaction (MOR) is reported. The well-defined PtBi@6.7%Pb nanocatalyst exhibits 4.0 and 7.4 times higher mass activity than PtBi nanoplates and commercial Pt/C catalyst toward MOR in the alkaline electrolyte at 30 degrees C. Meanwhile, it also achieves a record-high mass activity of 51.07 A mg(Pt)(-1) at direct methanol fuel cells operation temperature of 60 degrees C. DFT calculations reveal that the introduction of Pb oxyhydroxide on the surface not only promotes the electron transfer efficiency but also suppresses the CO poisoning effect, and the efficient p-d coupling optimizes the electroactivity of PtBi@6.7%Pb nanoplates toward the MOR process with low reaction barriers. This work offers a nanoengineering strategy to effectively construct and modulate multimetallic nanocatalysts to improve the electroactivity toward the MOR in future research.


I am an author on this paper
Click your name to claim this paper and add it to your profile.


Primary Rating

Not enough ratings

Secondary Ratings

Scientific rigor
Rate this paper


Article Chemistry, Multidisciplinary

Enabling Efficient Photocatalytic Hydrogen Evolution via In Situ Loading of Ni Single Atomic Sites on Red Phosphorus Quantum Dots

Guangri Jia, Mingzi Sun, Ying Wang, Xiaoqiang Cui, Bolong Huang, Jimmy C. C. Yu

Summary: A brand-new type of photocatalyst (Ni-RPQD) is proposed by loading Ni single atoms on the P vacancy defects of the RP quantum dots, achieving efficient hydrogen production. The Ni-P sites act as electron antennas, resulting in a high hydrogen production rate, which is 224 times higher than that of the original RPQD and competitive with non-noble metal-based SAC photocatalysts. Theoretical explorations reveal that atomically dispersed Ni atoms lower the energy barrier for electron transfer, leading to enhanced water adsorption and faster dissociation for more efficient H2 generation.


Article Chemistry, Multidisciplinary

Balancing Activity and Stability in Spinel Cobalt Oxides through Geometrical Sites Occupation towards Efficient Electrocatalytic Oxygen Evolution

Li An, Hong Zhang, Jiamin Zhu, Shibo Xi, Bolong Huang, Mingzi Sun, Yong Peng, Pinxian Xi, Chun-Hua Yan

Summary: Designing active and stable oxygen evolution reaction catalysts is crucial for various energy conversion devices. By introducing Ni and Mn elements and optimizing the geometrical structure, the catalyst surface can be modulated from oxygen-excess to oxygen-deficiency, resulting in excellent OER activity and long-term stability.


Article Chemistry, Multidisciplinary

Near-unity electrochemical conversion of nitrate to ammonia on crystalline nickel porphyrin-based covalent organic frameworks

Fang Lv, Mingzi Sun, Yongpan Hu, Jie Xu, Wei Huang, Na Han, Bolong Huang, Yanguang Li

Summary: Electrochemical nitrate reduction is a promising technology for the fixation of atmospheric N2 and the removal of nitrate from industrial wastewater. However, efficient and low-cost electrocatalysts are still lacking. In this study, a two-dimensional nickel porphyrin-based covalent organic framework (COF) was demonstrated as a potential candidate for nitrate reduction. The COF exhibited high selectivity, production rate, turnover frequency, and stability, and can be coupled with the oxygen evolution reaction for high-efficiency full-cell electrolysis. Theoretical computations revealed the stable adsorption of nitrate on nickel centers and the lowering of the energy barrier for the rate-determining step.


Article Chemistry, Multidisciplinary

Cooperative Rh-O5/Ni(Fe) Site for Efficient Biomass Upgrading Coupled with H2 Production

Lingyou Zeng, Yanju Chen, Mingzi Sun, Qizheng Huang, Kaian Sun, Jingyuan Ma, Jiong Li, Hao Tan, Menggang Li, Yuan Pan, Yunqi Liu, Mingchuan Luo, Bolong Huang, Shaojun Guo

Summary: Efficient and durable bifunctional catalysts have been designed for the co-production of biomass-upgraded chemicals and sustainable hydrogen through the oxidation of 5-hydroxymethylfurfural (HMF) and the evolution of hydrogen. Atomic-scale cooperative adsorption centers on Rh-O-5/Ni(Fe) atomic sites enable highly active and stable catalysis in alkaline conditions. The catalyst exhibits low cell voltage and excellent stability in an integrated electrolysis system.


Article Chemistry, Multidisciplinary

Cu-Co Dual-Atom Catalysts Supported on Hierarchical USY Zeolites for an Efficient Cross-Dehydrogenative C(sp2)-N Coupling Reaction

Tianxiang Chen, Wenhua Yu, Ching Kit Tommy Wun, Tai-Sing Wu, Mingzi Sun, Sarah J. Day, Zehao Li, Bo Yuan, Yong Wang, Mingjie Li, Zi Wang, Yung-Kang Peng, Wing-Yiu Yu, Kwok-Yin Wong, Bolong Huang, Taoyuan Liang, Tsz Woon Benedict Lo

Summary: A cross-coupling reaction via dehydrogenative route over heterogeneous solid atomic catalysts provides practical solutions for the economic and sustainable development of simple organic substrates. However, the limited molecular definition of many solid catalysts hampers the current utilization of this technology. In this study, Cu-M dual-atom catalysts supported on hierarchical USY zeolite were developed to efficiently mediate dehydrogenative cross-coupling of unprotected phenols with amine partners. The reaction showed over 80% isolated yields over Cu-Co-USY, which exhibited superior reactivity compared to Cu1 and other Cu-M analogues. This research offers critical insights into the engineering of next-generation solid atomic catalysts with complex reaction steps.


Article Chemistry, Physical

Stable all-solid-state Li-Te battery with Li3TbBr6 superionic conductor

Zhichao Zeng, Xiaomeng Shi, Mingzi Sun, Hongtu Zhang, Wei Luo, Yunhui Huang, Bolong Huang, Yaping Du, Chun-Hua Yan

Summary: Rare-earth halide solid electrolytes (HSEs) have become a promising research area for all-solid-state lithium batteries due to their favorable electrochemical and mechanical properties. However, only a few high-performance HSEs have been reported so far. In this study, a vacuum evaporation-assisted method was used to synthesize Li3TbBr6 (LTbB), a RE-HSE, with an impressive ionic conductivity of 1.7 mS center dot cm(-1), wide electrochemical window, and good formability. A solid Li-Te battery based on LTbB showed excellent cycling stability for up to 600 cycles, surpassing previous reports. Various in situ and ex situ characterizations were conducted to investigate the discharge/charge processes of Li-Te batteries. Theoretical calculations revealed that the direct [octahedral]-[octahedral] ([Oct]-[Oct]) pathway played a dominant role in Li ion migrations in the electrolyte, with efficient electron transfer at the Tb sites and unaffected Li 2s orbitals during migration, resulting in a low activation barrier. The successful fabrication and application of LTbB offer a competitive solution for solid electrolytes in all-solid-state lithium batteries and highlight the potential of RE-based HSEs in energy devices.


Article Chemistry, Physical

Atomically dispersed indium and cerium sites for selectively electroreduction of CO2 to formate

Zhong Liang, Lianpeng Song, Mingzi Sun, Bolong Huang, Yaping Du

Summary: In this study, novel single-atom InCe/CN catalysts were successfully prepared on a nitrogen-doped carbon matrix. Both AC-HAADF-STEM images and EXAFS spectra confirmed the well-dispersed In and Ce atoms. The prepared InCe/CN catalysts exhibited high Faradaic efficiency (77%) and current density (j(HCOOH)) for HCOOH formation in CO2 reduction reaction. Theoretical calculations showed that the introduced Ce single atom sites not only promoted electron transfer, but also increased the selectivity towards HCOOH formation by optimizing the In-5p orbitals. This work extends the design of single-atom catalysts to main group and Ln metals, providing more potential applications.


Article Chemistry, Physical

Strong Electronic Coupling Effects at the Heterojunction Interface of SnO2 Nanodots and g-C3N4 for Enhanced CO2 Electroreduction

Qian Zhang, Mingzi Sun, Chen-Yue Yuan, Qi-Wen Sun, Bolong Huang, Hao Dong, Ya-Wen Zhang

Summary: Constructing surface/interface structures is crucial for enhancing the performance of CO2 reduction catalysts. In this work, we report a 0D/2D heterojunction structure of SnO2 nanodots confined on g-C3N4 nanosheets, which promotes CO2 conversion to formate. The SnO2/g-C3N4 heterojunction exhibits high activity and stability, with a Faradic efficiency of 91.7% at -0.88 V vs RHE, due to strong metal oxide-support interactions and efficient electron transfer.


Article Chemistry, Physical

Atomscopic of ripple origins for two-dimensional monolayer transition metal dichalcogenides

Haitao Yu, Mingzi Sun, Xiao Wu, Cheuk Hei Chan, Bolong Huang, Zhong Lin Wang

Summary: Comprehensive theoretical studies on monolayer WSe2 reveal the sensitivity of its properties to ripple structures and demonstrate the significant role of ripples in optimizing optoelectronic performance.


Review Chemistry, Inorganic & Nuclear

Recent advances and strategies of electrocatalysts for large current density industrial hydrogen evolution reaction

Tong Wu, Mingzi Sun, Hon Ho Wong, Cheuk Hei Chan, Lu Lu, Qiuyang Lu, Baian Chen, Bolong Huang

Summary: The urgent need for sustainable energy resources has led to research on highly efficient electrocatalysts for the hydrogen evolution reaction (HER). However, most catalysts reported have only been evaluated under small current density and acidic conditions, while industrial HER requires higher current density and an alkaline medium. Therefore, recent efforts have focused on fulfilling the requirements for large current density and durability in alkaline conditions, as well as large-scale fabrication of the electrocatalysts and electrodes. This review provides significant insights into the future development of practical HER electrocatalysts.


Article Chemistry, Applied

High-entropy alloy metallene for highly efficient overall water splitting in acidic media

Dan Zhang, Yue Shi, Xilei Chen, Jianping Lai, Bolong Huang, Lei Wang

Summary: This study successfully prepared IrPdRhMoW HEA metallene catalyst, which exhibits extraordinary catalytic performance in acidic environments. It outperforms commercial catalysts and other noble metal-based catalysts in terms of hydrogen and oxygen evolution overpotentials. Moreover, it maintains excellent electroactivity and structural stability after prolonged water splitting.


Article Green & Sustainable Science & Technology

Tailoring the Electronic Structure of Ir Alloy Electrocatalysts through Lanthanide (La, Ce, Pr, and Nd) for Acidic Oxygen Evolution Enhancement

Shuai Zhang, Mingzi Sun, Leilei Yin, Siyuan Wang, Bolong Huang, Yaping Du, Chun-Hua Yan

Summary: A solid-phase synthesis strategy is developed for the preparation of Ir-Ln (Ln = La, Ce, Pr, Nd) alloy nanoparticles on carbon supports, which serve as superior acidic OER catalysts. Among them, Ir2Pr alloy catalyst exhibits a maximum mass activity of 2.10 A mg(Ir)(-1) at 300 mV overpotential and stability over 200 h at 10 mA cm(-2) in 0.5 m H2SO4, which is 9.5 and 20 times higher compared to pure Ir nanoparticles. Theoretical calculations confirm the correlation between the OER performances and the rare earth elements in the alloy.


Article Green & Sustainable Science & Technology

Strong Electron-Phonon Coupling Induced Self-Trapped Excitons in Double Halide Perovskites

Baian Chen, Rui Chen, Bolong Huang

Summary: Double halide perovskites have shown potential for self-trapped exciton (STE) luminescence, but the formation mechanism of STEs in these materials is still unclear. The electronic structures, exciton characteristics, electron-phonon coupling performances, and geometrical configuration of a series of double halide perovskites (Cs2BBCl6)-B-1-Cl-2 (B-1 = Na+, K+; B-2 = Al3+, Ga3+, In3+) are theoretically studied. The Ga-series double halide perovskites exhibit stronger electron-phonon coupling strength, and Cs2NaGaCl6 shows a high and effective Huang-Rhys factor of 36.21. The Jahn-Teller distortion induced by hole-trapping after excitation is responsible for the existence of STEs in Cs2NaGaCl6. This study improves the understanding of STEs and provides guidance for advanced solid-state phosphor design.


Article Chemistry, Multidisciplinary

Adjacent Fe Site boosts electrocatalytic oxygen evolution at Co site in single-atom-catalyst through a dual-metal-site design

Changli Chen, Mingzi Sun, Fang Zhang, Haijing Li, Mengru Sun, Pin Fang, Tinglu Song, Wenxing Chen, Juncai Dong, Brian Rosen, Pengwan Chen, Bolong Huang, Yujing Li

Summary: A Co-Fe dual-atomic catalyst with optimized intrinsic oxygen evolution reaction (OER) performance was designed, where the role of individual metal sites was investigated. The optimized catalyst exhibited OER activity with an overpotential of 240 mV and turnover frequency of 146 s(-1) (10 mA cm(-2)). The interplay between Co and Fe metal sites was identified as the key factor for improved OER performance, with Co sites acting as active sites and adjacent Fe sites serving as co-catalytic sites.


No Data Available