Nature Communications
·
2026
·
IF 18.1
Zhao Dafu,Tang Zisheng,Liu Jinfeng,Hu Zhiyi,Yin Zhiwen,Lv Jieheng,Liao Xiaobin,Wang Xiaoqian,Liu Yingfei,Liu Damin,Chen Lihua,Su Bao-Lian,Zhao Dongyuan,Liu Yong
Practical electrochemical energy conversion requires electrocatalysts that coordinate multiple elementary steps at spatially distinct active sites, yet atomic-level control of such site-specific reactivity within a single heterogeneous particle remains challenging. Here we propose and realize atomic-scale gradient strain as a design concept for heterogeneous electrocatalysis. Using Pd@Pt core-shell tetrahedra as a model system, we construct a continuous lattice-strain gradient across individual 3–4 atomic-layer Pt {111} epitaxial shells, where lattice-mismatch-driven compression relaxes from edges to center regions. This single-particle strain gradient, spanning approximately −8% to −2%, spatially links *O 2 activation at highly compressed sites with *OH weakening at moderately compressed sites through kinetically accessible intermediate redistribution. The catalysts exhibit competitive oxygen reduction reaction performance, with mass and specific activities of 2.19 A mg Pt ⁻ 1 and 3.01 mA cm⁻ 2 at 0.9 V vs reversible hydrogen electrode, while retaining 91% activity after 20 k cycles. In membrane electrode assemblies, they achieve 0.57 A mg Pt ⁻ 1 , and peak power densities of 2.10 W cm⁻ 2 in H 2 − O 2 and 1.16 W cm⁻ 2 in H 2 −air, with over 90% performance retention after 20 k cycles.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lianming Zhao,Jinghao Zhang,Chang Xu,Shouao Li,Yanfu Tong,Guangkun Yan,Wenxuan An,Pengyun Liu,Xuejin Li,Guang Zhao,Jing Xu,Wei Xing
Sub-3 nm PtRuNiCoCu HEA NPs were synthesized via a nanoreactor-confined strategy. • Mesoporous NHCS confinement ensures a uniform single-phase FCC HEA structure. • The spatially separated dual sites for H* and OH* optimize HOR kinetics. • The catalyst shows high alkaline HOR mass activity (3329.32 A g −1 ) and CO tolerance. To address the sluggish hydrogen oxidation reaction (HOR) kinetics in anion exchange membrane fuel cells (AEMFCs), a PtRuNiCoCu@NHCSs electrocatalyst is developed through the in situ synthesis of ultrasmall (<3 nm) PtRuNiCoCu high-entropy alloy nanoparticles (HEA NPs) confined within hollow mesoporous nitrogen-doped carbon spheres (NHCSs), using a vapor-infusion-assisted pyrolytic reduction strategy. The nanoreactor confinement provided by NHCSs suppresses phase separation, yielding a single-phase face-centered cubic structure, ensures uniform dispersion and stability of the HEA NPs. The ultrasmall nanoparticle size provides a large electrochemically active surface area and abundant accessible active sites. Electronic interactions among the multimetallic components create electron-rich and electron-deficient regions on the HEA surface, forming spatially separated dual-active sites for H* and OH*, which mitigates competitive adsorption and generates a broad distribution of adsorption energies. This establishes multiple low-energy reaction pathways, collectively lowering the HOR barrier, while simultaneously weakening CO binding. These synergistic structural and electronic effects endow the PtRuNiCoCu@NHCSs catalyst with outstanding alkaline HOR performance, achieving a mass activity of 3329.32 A g −1 Pt+Ru and an exchange current density of 9.43 mA cm −2 , along with remarkable durability and CO tolerance. This study provides both a general synthesis route for ultrasmall HEAs and a mechanistic framework for designing advanced AEMFC electrocatalysts. Download: Download high-res image (160KB) Download: Download full-size image
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 29
·39793-39801
·
IF 7.8
Chen Wengang,Cheng Haocong,Lyu Jiahui,Gong Lei,Chen Cheng,Jiang Zhijun,Sang Wei,Mu Shichun,Kou Zongkui
Pt-based alloy catalysts have been established as highly
active
and robust oxygen reduction reaction (ORR) electrocatalysts in the
practical proton exchange membrane fuel cell (PEMFC). Nevertheless,
fabricating such catalysts with low Pt loading via low-cost, solvent-free,
and size-controllable synthetic protocols remains an open space to
be explored. Herein, we combined an all-solid-state synthesis of ZIF-8
precursor with a direct confined pyrolysis for the uniform anchoring
of PtFe alloy nanoparticles on nitrogen-doped carbon derived from
ZIF-8 (PtFe/NC). The resulting PtFe/NC catalyst with only 1.59 wt
% Pt exhibits a remarkable half-wave potential of 0.897 V and a mass
activity of 2.34 A mg Pt –1 (@0.90 V, iR -free), outperforming commercial 20 wt % Pt/C (0.14 A
mg Pt –1 ) by a factor of 17. We have confirmed
that Fe doping can effectively restrict the growth of Pt particles.
Meanwhile, integrating Fe atoms into the Pt lattice results in a 3.6%
lattice compression, which correspondingly downshifts the d-band center
and optimizes the adsorption strength toward reaction intermediates,
thereby facilitating oxygen release and significantly enhances the
catalytic activity.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 31
·42780-42788
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IF 7.8
Zou Lie,Huang Xiao-Yan,Zhang Yi,A Yao-Lin,Xu Qing-Chi,Chen Bing-Hui,Liu Jinxuan,Zhang Hua,Li Jian-Feng
Understanding the molecular origins of oxygen reduction reaction (ORR) activity on Pt-based catalysts is essential for the rational design of high-performance electrocatalysts. Herein, by combining electrochemical measurements with in situ shell-isolated nanoparticle-enhanced Raman spectroscopy (SHINERS), we systematically investigate the ORR pathway on Pt-based alloy nanocatalysts incorporating different transition metals to elucidate how surface oxygenated intermediates dictate ORR activity. Among the catalysts examined, PtNi exhibited higher activity than PtFe, PtCo, and commercial Pt/C, underscoring the pronounced sensitivity of intrinsic ORR activity to alloy composition. Potential-dependent in situ Raman spectra, corroborated by isotopic labeling, directly identified *OOH as a key ORR intermediate and established a clear correlation between its vibrational frequency and catalytic activity. The results suggest that Ni alloying may modify the electronic environment of Pt, thereby weakening the Pt-O interaction, optimizing the adsorption state of the kinetically relevant *OOH intermediate, and consequently promoting ORR kinetics. This study establishes an effective spectroscopic platform for probing ORR intermediates on realistic electrocatalyst surfaces and offers molecular-level understanding of the activity enhancement in Pt-based alloy catalysts.
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RENEWABLE ENERGY
·
2026
·
IF 9.1
Qingtao Wang,Rongqian Li,Xingyong Li,Yiyang Zhao,Xueyan Jing,Jing Zhang,Na Liu,Senshen Yu,Xuexiang Fu,Phidsavard Keomeesay,Olajide-rasheed Olalekan,Yubao Chen
Renewable diesel derived from biomass offers a sustainable alternative to conventional fossil fuels, yet its efficient production under mild conditions remains challenging. Herein, we report a PdPtRuCuNi high-entropy alloy/TiO 2 catalyst synthesized via a facile one-pot solvothermal method for the photothermal decarboxylation of biomass-derived oils and fatty acids into diesel-range alkanes. Structural characterizations confirm the successful formation and uniform dispersion of multicomponent HEA particles on TiO 2 . The integration of PdPtRuCuNi alloy sites with oxygen-vacancy-rich TiO 2 creates a cooperative metal–oxide interface that promotes light-induced charge separation, accelerates interfacial electron transfer, and suppresses carrier recombination. Meanwhile, the HEA/TiO 2 interface facilitates H 2 activation, hydrogen spillover, and the adsorption/activation of oxygenated intermediates, thereby enhancing the decarboxylation pathway under mild photothermal conditions. As a result, the catalyst achieves complete conversion of oleic acid with 98.8% selectivity toward renewable diesel-range alkanes at 100 °C and 0.4 MPa H 2 within 3.5 h. Moreover, it retains 91.2% selectivity toward C 15 -C 17 alkanes after ten consecutive cycles, demonstrating excellent stability. This work establishes a high-entropy-alloy/oxide interfacial strategy for efficient photothermal biomass upgrading to renewable fuels.
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Nano-Micro Letters
·
2026
·Vol. 18
·期 1
·257
·
IF 38.5
Zhou Yin,Yin Kun,Zhang Tian,Feng Dongyu,Li Jiapei,Zhu Anquan,Lin Dewu,Xue Pan,Liu Yu,Liu Yongyu,Liu Kai,Liu Kunlun,Luan Chuhao,Yang Huawei,Chen Hou,Yao Yagang,Hong Guo
PtFe catalyst was rationally designed based on frontier molecular orbital theory to investigate orbital-level interactions for enhanced oxygen evolution reaction activity in Li–O 2 batteries.
The d z 2 – d z 2 orbital coupling between Fe and Pt leads to electron donation from Fe to Pt, increasing electron population in the Pt d z 2 orbital.
Excess electrons from the Pt d z 2 orbital occupy antibonding states with LiO 2 , weakening interaction strength and boosting oxygen evolution reaction kinetics.
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JOURNAL OF CATALYSIS
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2026
·
IF 6
Jie Wang,Feng Gao,Jilei Lin,Chunjuan Zhang,Meiqing Shen,Linghui Kong,Gurong Shen
Ammonia is emerging as a promising carbon-free energy carrier. The electrocatalytic ammonia oxidation reaction (AOR), highly structure-sensitive, exhibits exceptional activity on Pt nanocubes (NCs) with (100) facets. Yet, synthesis methods employing metal carbonyl capping agents inevitably introduce residual metals, whose catalytic effects are often neglected. Here, Pt NCs synthesized with Mo(CO) 6 were found to contain trace Mo both in the bulk and at the surface. Surface Mo species, partially oxidized to MoO x , substantially modify the electronic structure of Pt(100), lowering activation barriers for rate-determining AOR steps and enhancing resistance to nitrogen poisoning. These effects collectively boost AOR performance, enabling a direct ammonia fuel cell with a Pt-154 anode to achieve a peak power density of 26.7 mW cm −2 . These results reveal the overlooked impact of capping-agent-derived contaminants in AOR and point to the deliberate incorporation of heterometallic modifiers as a viable strategy for advanced electrocatalyst design.
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ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Shaohui Zhang,Qing Li,Suying Liu,Juan Luo,Yuke Gu,Xuanzhi Liu,Feng Liu,Pengfei Tan,Jun Pan
Defect fabrication is a practical nanosurface engineering to efficiently promote the oxygen reduction reaction (ORR) but remains a huge challenge. Herein, defect-rich ordered PtCu nanooctahedrons (D-PtCu-NOs) were prepared using Cl– as a shape-directing and etching agent. As a result, the D-PtCu-NOs catalyst achieves a mass activity of 1.147 A mgPt–1, which is 10.6-fold that of Pt/C. Meanwhile, the ordered and octahedral structures of the D-PtCu-NOs catalyst enable it to achieve an extremely high catalytic stability for 30,000 cycles. Convincingly, the D-PtCu-NOs catalyst also displays a higher peak power density and long-term durability than Pt/C in fuel cells. Besides, theoretical calculations reveal that the pore defects reduce the d-band center of Pt, lower the H2O formation barrier to boost the ORR activity, whereas the ordered structure inhibits the solubility of Pt and Cu, thereby improving the catalytic stability. This work highlights the importance of defect engineering for Pt-based nanocrystals to enhance the ORR.
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PHYSICAL CHEMISTRY CHEMICAL PHYSICS
·
2026
·
IF 3
Xiaolong Ma,Shujun Chen,Anqin Li,Wuying Chen,Mingze Hou,Kun Long,Gang Hu,Biao Qin
To address the insufficient activity, low noble metal utilization efficiency, and poor stability of transition metal-based catalysts in alkaline media, a PtFeCoNiMnMo high-entropy alloy (HEA) nanocatalyst with synergistic multi-d orbital hybridization was synthesized via a one-pot solvothermal method using glucose as a dispersant and an auxiliary reducing agent. Comprehensive characterization (XRD, TEM, XPS, and ICP-OES) confirmed its single face-centered cubic structure with lattice distortion (δ = 3.29%), homogeneous elemental distribution, and directional electron transfer-induced strong electronic interactions. Electrochemical tests in 1 M KOH showed exceptional alkaline hydrogen evolution reaction (HER) performance: 21 mV overpotential at 10 mA cm−2, 47.06 mV dec−1 Tafel slope, 2.455 s−1 TOF, and minimal charge-transfer resistance (5.39 Ω), outperforming control samples and commercial Pt/C. The catalyst exhibited outstanding stability with only 2.1% current decay after 50 h. Mechanistic studies indicated that the multi-d orbital electronic interactions in the alloy can regulate the adsorption capacities of H and OH species, thereby enhancing its alkaline HER catalytic activity.
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JOURNAL OF NANOBIOTECHNOLOGY
·
2026
·
IF 15
Wei Zhang,Yanan Zhou,Zijun Li,Zhaowen Wang,Fangzheng Zhu,Yaoyu Zou,Nianshuang Li,Cong He,Nonghua Lu,Xiaolei Wang,Yin Zhu
Helicobacter pylori (H. pylori) infection has emerged as a serious risk factor for global human health. Current antibiotic-based clinical eradication therapies still have many challenges, including inadequate drug permeability across the gastric mucus barrier, H. pylori biofilm-induced antibiotic resistance and recurrent infections, as well as gut dysbacteriosis. Herein, we report a probiotic-nanozyme hybrid system (LP@FeTA/CuPt), which is formed by coupling polyphenol-coated Lactobacillus plantarum (LP@FeTA) and CuPt nanozymes. LP@FeTA effectively penetrates the gastric mucus barrier via autokinetic movement, and facilitates the targeted delivery of CuPt nanozymes within H. pylori biofilms by "eating" extracellular polymeric substances (EPS). CuPt nanozymes respond to the acidic and H 2 O 2 -rich biofilm microenvironment to generate reactive oxygen species (ROS) and release Cu ions, thereby achieving multi-target eradication of biofilms by interfering with H. pylori flagellar self-assembly, urease activity, outer membrane function and energy metabolism. Importantly, LP@FeTA/CuPt can be degraded by transferrin at the infection site, allowing the released CuPt nanozymes to reactivate the antibacterial immune functions of macrophage, thus eliminating biofilm-escaped bacterioplankton to prevent recurrent infections. Notably, LP@FeTA/CuPt also modulates gut microbiota homeostasis. This study provides a promising non-antibiotic therapeutic strategy for H. pylori infection.
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JOURNAL OF POWER SOURCES
·
2026
·
IF 8.4
Zixuan Deng,Shuang Zhang,Fudong Li,Yue Zhu,Changsheng Shan,Yuanmeng Zhao
Rationally designing electrocatalyst/electrolyte interfaces with excellent active hydrogen supply capability is crucial for the hydrogen evolution reaction (HER), a core step in alkaline anion exchange membrane water electrolysis (AEMWE). Herein, phosphorus (P)-surface-coordinated PtFeCoCuMo quinary alloys are synthesized via a two-step wet-chemical method. P-induced d-p orbital hybridization enables the synergistic regulation of two key factors: it optimizes the hydrogen adsorption free energy (ΔG H∗ ) and water dissociation barrier (thermodynamic modulation), while tailoring the potential of zero charge (PZC) to accelerate proton transport (kinetic modulation). The optimized P 16 -PtFeCoCuMo catalyst exhibits outstanding alkaline HER activity, with a turnover frequency (TOF) 5-fold and 3-fold higher than those of commercial Pt/C and pristine PtFeCoCuMo alloy, respectively. This work overcomes thermodynamic and kinetic limitations simultaneously through heteroatom doping, providing a promising strategy for the design of high-performance alkaline HER catalysts.
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ACS Applied Materials & Interfaces
·
2026
·Vol. 18
·期 34
·46312-46321
·
IF 7.8
Wang Guangxia,Sun Xiuwei,Geng Ruyang,Xu Yong,Hu Tao,Qiu Zhenping
The commercialization of direct alcohol fuel cells (DAFCs) is severely hindered by sluggish anodic alcohol oxidation reaction kinetics and the high susceptibility of catalysts to deactivation. Traditional Pd/Pt-based catalysts suffer from difficult C−C bond cleavage and severe CO poisoning. To address these issues, we synthesize a pentametallic PdPtNiBiCo alloy consisting of interconnected nanoparticles via a facile one-pot oil-phase method, aiming to maximize electrochemically accessible surface sites and trigger robust multimetallic synergy. This architecture delivers an exceptional alkaline ethanol oxidation activity of 16.64 A mg −1 Pd+Pt , 12 and 19 times higher than those of commercial Pd/C and Pt/C, respectively. Furthermore, the catalyst exhibits robust antipoisoning durability over 4000 cycles and broad activity for methanol and ethylene glycol oxidation. Density functional theory calculations reveal that multimetallic synergy effectively modulates the d-band center of the active sites. Density functional theory calculations reveal that multimetallic synergy tunes the electronic structure of the active sites, optimizes the adsorption of key intermediates, and lowers the thermodynamic energy requirements for C−C bond cleavage and CO oxidation, thereby facilitating both the C1 and C2 pathways of ethanol oxidation. This work addresses the key limitation of traditional Pd/Pt-based catalysts and provides an effective strategy for designing high-performance universal DAFC anodes.
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