CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Yan Tong,Pengkai Xing,Wenbo Ruan,Xiaopeng Wang,Rui Zhang,Weixin Lv,Muhammad Ikram,Xue Bai,Qin Guo,Keying Shi
Room-temperature (RT) detection of NO 2 remains challenging because low-temperature operation often limits surface reactivity and charge-transport modulation. Here, a noble-metal-decorated hollow cage-like oxide is constructed by integrating a template-assisted route with hydrothermal processing, yielding a cauliflower-like architecture with a high specific surface area and abundant, accessible adsorption sites for NO 2 capture. Surface decoration further enriches oxygen vacancies and enhances the oxygen storage capacity, promoting oxygen activation and NO x surface chemistry under ambient conditions. Meanwhile, the formation of a Schottky barrier between Pd and CeO 2 enhances the conductivity and electron mobility of the composite. As a result, the chemiresistive sensor delivers a response of 32.84 toward 100 ppm NO 2 at room temperature, with a 3 s response and 15 s recovery, while maintaining good selectivity, repeatability, and long-term stability. The device further achieves a 30 ppb detection limit, highlighting this hollow, vacancy-rich microcage platform as an effective strategy for low-power NO 2 monitoring. This work provides a generalizable interface and defect engineering strategy for next-generation RT NO 2 sensors.
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ACTA PHYSICO-CHIMICA SINICA
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2026
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IF 13.5
Shunyi Tang,Heng Guo,Bo Yu,Juan Liu,Linqiu Li,Haoran Wu,Weijun Tian,Fengying Zhang,Ying Zhou
The electrocatalytic reduction of nitrate to ammonia (NO 3 − RR) represents a promising strategy for sustainable nitrogen cycling and the valorisation of wastewater. Its practical implementation, however, is limited by sluggish kinetics, stemming from inefficient proton delivery during the multi-step electron/proton transfer, which restricts both ammonia selectivity and yield. In this work, we report a Pd-Ru bimetallic catalyst supported on nickel foam (Pd-Ru/NF), which functions through a hydrogen shuttle relay mechanism between dual-function sites. Combined experimental and theoretical analyses indicate that Pd sites are principally responsible for nitrate activation and hydrogenation, while adjacent Ru sites efficiently cleave water to supply active hydrogen species (H*). This cooperative interaction creates a dynamic hydrogen-transfer network, enabling rapid and directed proton delivery to reaction intermediates. The relay process not only accelerates the critical hydrogenation steps but also effectively suppresses the competing hydrogen evolution reaction (HER). Consequently, the Pd-Ru/NF electrode attains a notable ammonia yield of 1.77 mmol cm −2 h −1 with a Faradaic efficiency of 85.95% at −1.4 V vs. RHE. This study establishes a novel catalyst design paradigm based on the management of interfacial hydrogen transfer, providing a general strategy to enhance the efficiency of proton-coupled electrocatalytic transformations.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Saisai Zhang,Yi Zheng,Bo Zhang,Bowen Zhang,Na Luo,Yan Wang
Since nitrogen dioxide (NO 2 ) is an air pollutant that can seriously harm human health, developing high-performance gas sensors capable of efficiently detecting nitrogen dioxide at room temperature is of great significance for environmental monitoring and health protection. In this work, we synthesized hierarchical spherical MoS 2 with a high specific surface area via a hydrothermal method and uniformly loaded Pd nanoparticles onto its surface through an in-situ reduction strategy, successfully constructing a Pd/MoS 2 composite material. Characterization techniques including SEM, TEM，XPS confirmed the successful loading of Pd nanoparticles and the electronic interaction between Pd and MoS 2 . Experimental results demonstrate that the 1% Pd/MoS 2 composite exhibits optimal sensing performance toward NO 2 at room temperature: a high response value (Rg/Ra) of 9.33 toward 10 ppm NO 2 , along with excellent selectivity, repeatability, and long-term stability. Density Functional Theory (DFT) calculations further elucidated the enhancement mechanism: the introduction of Pd significantly increased the adsorption energy of NO 2 on the material surface (from −0.253 eV to −1.41 eV), thereby greatly improving the sensor's sensitivity and response kinetics. This research provides an effective material design strategy and theoretical foundation for developing high-performance, low-power-consumption room-temperature NO 2 gas sensors.
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SmartMat
·
2026
·Vol. 7
·期 2
·e70073
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IF 14.3
Mengjie Xu,Min Hao,Jing Yu,Junfeng Du,Shuai Zhang,Haibin Chu,Yaping Du
The electrocatalytic nitrate reduction reaction (NO 3 RR) provides a sustainable route for nitrogen pollution remediation and ammonia production under ambient conditions. However, the process involves sluggish multi-electron/proton transfer and suffers from competing hydrogen evolution (HER) which severely limits efficiency and selectivity. Herein, we construct a Pd x -CeO 2 /C composite catalyst, in which strong interactions between Pd and CeO 2 induce interfacial electronic redistribution, thereby effectively modulating the Pd electronic structure. This interfacial coupling enhances water dissociation, accelerates the generation of reactive *H, and promotes its spillover from Pd to CeO 2 . In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) confirms that hydrogen spillovers facilitate stepwise hydrogenation of intermediates while suppressing HER. Density functional theory calculations further reveal that Pd-Ce interactions inhibit HER and enable N─O side-on adsorption, shifting the potential-determining step and lowering the reaction barrier, thus boosting electrocatalytic activity. As a result, the optimized 5 wt.% Pd-CeO 2 /C delivers a Faradaic efficiency of 98.0% for ammonia at −0.4 V (vs. RHE), and achieves an ammonia yield rate of 4.17 mmol/(mg Pd ∙h) at −0.6 V. This work offers new insights into the application of interfacial engineering for efficient electrocatalytic ammonia synthesis.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Yuxin Tang,Xinyi Yang,Lingyu Zeng,Bili Tan,Fei Qi,Bo Feng,Liang Wang,Guangbo Che
Precise atomic-scale interface engineering across the entire pH range remains a formidable challenge for photocatalytic H 2 evolution. Herein, hexamethylenetetramine (HMT) is introduced as a bifunctional surface modifier that spontaneously constructs Pd-N coordination bridges on g-C 3 N 4 . The interfacial Pd-N bonds collectively down-shift the N-p-band center away from the Fermi level, break intrinsic surface charge symmetry of C/N atoms, and fully expose the originally buried N active sites, thereby steering the hydrogen adsorption free energy (|ΔG H* |) toward thermoneutral. Simultaneously, the Pd-N bond confines Pd cluster growth to ∼5 nm, doubling specific surface area and enriching edge active sites that serve as primary proton reduction centers. Transient photoelectric voltage results reveal that the Pd-N electron transfer channel shortens the carrier transfer path and prolongs photoelectron lifetime, enabling quantitative electron delivery under acidic, neutral, and alkaline environments. As a result, the Pd-CN-HMT sample presents an efficient H 2 evolution rate across the entire pH window. This work advances the field by providing a versatile ligand-based strategy to precisely tailor the interfacial electronic structure via strong chemical bonding, offering a distinct and scalable solution for constructing high-performance pH-universal photocatalysts.
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RARE METALS
·
2026
·Vol. 45
·期 10
·e70671
·
IF 12.1
Zhidan Wang,Rui Li,Yawen Wang,Yunfang Wang,Caimei Fan,Jianxin Liu,Shan Gao,Jiancheng Wang
en This link goes to a English section zh This link goes to a Chinese section Photocatalytic acetylene (C 2 H 2 ) semihydrogenation is a green route for ethylene (C 2 H 4 ) production, yet the activity–selectivity trade-off caused by imbalanced adsorption/activation of reactants and products remains a core challenge. Herein, we realize precise regulation of Pd oxidation states (Pd 0 , Pd δ + , and Pd 2+ ) on anatase TiO 2 nanocubes via a mild reduction strategy, fabricating a Pd δ + /TiO 2 photocatalyst with intermediate valence of Pd sites. Systematic characterizations and theoretical calculations reveal that Pd δ + optimizes the d-π/d-π* orbital interactions between Pd and C 2 H 2 /C 2 H 4 , achieving a moderate adsorption strength that balances efficient C 2 H 2 activation and rapid C 2 H 4 desorption. Pd 0 causes overadsorption/overhydrogenation, whereas Pd 2+ leads to weak substrate activation. Consequently, Pd δ + /TiO 2 achieves nearly 100% C 2 H 2 conversion and ∼90% C 2 H 4 selectivity, with a record-high turnover number (TON) of ∼4.1 × 10 4 and excellent cycling stability. This work clarifies the electronic mechanism of Pd valence engineering in carrier dynamics and modulating orbital hybridization, providing a new strategy for the rational design of C 2 H 2 semihydrogenation photocatalysts. 摘要 en This link goes to a English section zh This link goes to a Chinese section 光催化乙炔(C 2 H 2 )半加氢是一种制备乙烯(C 2 H 4 )的绿色路径,但反应物与产物吸附与活化不均衡引发的活性-选择性权衡问题仍是核心难题。本文通过温和还原策略,在锐钛矿二氧化钛纳米立方体上实现钯氧化态(Pd 0 、Pd δ + 、Pd 2+ )的精准调控,制备出活性位点为中间价态钯的 Pd δ + /TiO 2 光催化剂。系统表征与理论计算结果表明,Pd δ + 能够优化钯与C 2 H 2 /C 2 H 4 之间的d-π/d-π* 轨道相互作用,形成适中的吸附强度,兼顾高效活化乙炔与乙烯快速脱附, Pd 0 会造成吸附过强并引发过度加氢,而Pd 2+ 对底物活化能力较弱。因此,Pd δ + /TiO 2 可实现接近 100% 的乙炔转化率和约 90% 的乙烯选择性,周转数(TON)高达4.1 × 10 4 ,同时具备优异的循环稳定性。该研究阐明了调控钯价态对载流子动力学及轨道杂化进行调控的电子作用机制,为乙炔半加氢光催化剂的合理设计提供了新思路。
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
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IF 8.3
Haoshuang Zhang,Tianshuang Wang,Liupeng Zhao,Xueying Kou,Peng Sun,Geyu Lu
The detection of flammable and explosive methanol (CH 3 OH) at room temperature remains challenging for semiconductor gas sensors, severely restricting their practical applications due to low sensitivity, high detection limit, and poor selectivity. Herein, we report a UV-activated gas sensor based on Pd-doped W 18 O 49 that exhibits high response to CH 3 OH along with rapid response/recovery times (169 s/346 s), and low detection limit (100 ppb), representing one of the best performances reported to date for room-temperature CH 3 OH sensing. The enhanced room-temperature sensing performance under UV illumination is attributed to the effective electron-transport pathway within nanowires, doping-induced energy band structure optimization, high adsorption capacity on defect-rich surface, and facilitated CH 3 OH dehydrogenation, as verified by density functional theory (DFT) calculations and comprehensive optical and electrical characterizations. To demonstrate practical application, a portable sensing and monitoring system was developed, enabling successful real-time indoor air quality assessment with an alarm function. This work provides a viable and efficient solution for room-temperature volatile organic compounds monitoring.
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ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Ou Wang,Leiyu Diao,Ping Li,Youyou Feng,Dong Cheng,Yaqiong Su,Jing Wei
Pd-based nanoparticles have been widely employed to enhance H 2 sensing performance due to their strong capability for H 2 adsorption and dissociation. However, strong Pd–H* interactions hinder the hydrogen spillover process, while pronounced CO adsorption results in poor selectivity. Herein, we propose a Pt–Pd single-atom alloy (SAA) sensitization strategy that creates electron-deficient Pd δ+ sites to modulate the interaction between Pd and gas molecules. As a proof of concept, Pt 1 Pd SAA is deposited on commercial SnO 2 to fabricate H 2 sensors. The resulting device achieves an ultra-low detection limit (21 ppb), short response and recovery time (0.8 s and 5.9 s), excellent selectivity and enhanced CO resistance, outperforming traditional Pd nanoparticles, PtPd alloy sensitizers modified SnO 2 gas sensors, and commercial H 2 sensors. Mechanistic studies establish that atomic Pt induces electron-deficient Pd δ+ sites, achieving atomic-scale decoupling of hydrogen activation from CO adsorption, which enables barrierless hydrogen spillover and inherently CO-resistance H 2 sensing, with CO back-donation suppressed by nearly 50%. This study presents a robust SAA sensitization strategy that leverages atomic-level modification-induced electronic structure modulation to overcome the sensitivity-selectivity trade-off, demonstrating its promise for next-generation H 2 sensors.
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MATERIALS CHEMISTRY AND PHYSICS
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2026
·
IF 5.2
XueLi Li,Yu Wang,Chaoyang Ma,Hengjie Li,Yantu Zhang,Ruiling Lu
Hollow mesoporous silica nanospheres (HMSS) with radially ordered mesopores and isolated cavities were synthesized via a selective etching method. The surface of HMSS was functionalized with amino groups using 3-aminopropyltriethoxysilane (APTES) to obtain HMSS-NH 2 . Subsequently, palladium nanoparticles, palladium nanoparticles with an approximate mean size of 1.9 nm were deposited onto HMSS-NH 2 by means of an incipient wetness impregnation-reduction technique, yielding the Pd/HMSS-NH 2 catalyst. A systematic evaluation was conducted to assess the catalytic performance of the material in formic acid (FA) dehydrogenation. The findings indicate that the optimized Pd/HMSS-NH 2 catalyst (equipped with 10 wt% Pd content and 3 mL APTES) manifests an initial turnover frequency (TOF) of 3600 h −1 at 323 K for FA dehydrogenation, exhibiting an apparent activation energy as low as 29.3 kJ/mol. The full FA conversion and >99.99% H 2 selectivity were achieved under mild conditions. Furthermore, the catalyst retains good activity after five cycles. The superior activity of Pd/HMSS-NH 2 is attributable to the synergistic effect of the distinctive hollow mesoporous construction of HMSS and the surface amino groups, which effectively stabilize the active Pd nanoparticles. This investigation presents a novel strategy for engineering functional heterogeneous catalysts for hydrogen generation from FA.
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Shuo Han,Xu-bin Wang,Qian-cheng Sun,Wen-feng Yang,Fei Xiao
Simple immersion surface Pd alloying modification yields high-strength Cu-Cu bonding. • Disorder-to-order transformation offers extra driving force unlike inert Pd layer. • Lattice distortion & atomic pinning give 160 MPa shear strength at 76% bonding ratio. • Glycerol reduces oxide to nanocrystals and prevents oxidation during bonding in air. Low-temperature Cu-Cu thermal-compression bonding is essential for three-dimensional integrated circuits (3D ICs) to achieve high-density vertical interconnects. The key scientific challenge lies in achieving sufficient atomic interdiffusion at temperatures below 250 °C, where volume diffusion is sluggish and native oxides impede metal‑to‑metal contact. Here, this challenge is overcome by a simple galvanic displacement reaction that forms a disordered Cu-Pd surface alloy, followed by glycerol‑assisted bonding. This surface engineering simultaneously reduces roughness, raises surface energy, refines grains, and introduces micro-strain, while glycerol removes residual oxides in-situ and protects the interface from re-oxidation. These modifications accelerate atomic diffusion, and the exothermic defect annihilation and disorder-to-order transformation further lowers the diffusion barrier. Consequently, Pd‑displaced samples exhibit high shear strength and bonding ratio, and Kirkendall voids shrink under bonding conditions, potentially mitigating electrical concerns. The measured strength exceeds predictions from the bonding area alone due to solid‑solution hardening and lattice distortion. This work provides a simple, selective, and industrially viable route for low‑temperature Cu-Cu and hybrid bonding, offering a new surface‑alloying strategy with potential applicability to advanced packaging. Simple immersion surface alloying with glycerol reduction and protection achieves high‑strength Cu‑Cu bonding in air via abundant grain boundaries, disorder‑to‑order transformation and lattice distortion (exceeding estimated bulk Cu shear strength), while Kirkendall voids shrink with bonding durations to reduce potential electrical concerns. Download: Download high-res image (408KB) Download: Download full-size image
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CRYSTENGCOMM
·
2025
·
IF 2.6
hanchi Ma,Hao Wang,Xiya Yan,Bin Liu,Jianhui Yang
Au@Pd@Pt core-shell nanoparticles (CSNs) with mesoporous structures and nanocavities were synthesized through a seed-mediated growth method. The process involved the initial formation of Au@Pd CSNs via the reduction of PdCl₄²⁻ by ascorbic acid (VC), followed by a reduction of PtCl62- by VC and a galvanic replacement reaction between the Pd shell and PtCl₆²⁻. The galvanic replacement reaction is a critical step in the formation of Au@Pd@Pt CSNs featuring distinctive void in the mesoporous structures. The electrocatalytic performance of the as-synthesized Au@Pd@Pt CSNs for the ethanol oxidation reaction (EOR) was systematically evaluated. Due to the unique hierarchical structure featuring both mesoporosity and internal nanocavities, the Au@Pd@Pt CSNs exhibited significantly enhanced electrocatalytic activity compared to Au@Pd CSNs, Au@Pt CSNs, and commercial Pd/C catalysts. This work presents a facile strategy for constructing hierarchical core-shell nanostructures, demonstrating considerable potential for application in electrocatalytic ethanol oxidation.
研究领域:
纳米材料
·
电催化
·
能量转换
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燃料电池
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纳米技术
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2025
·
IF 3.9
Zhiyuan Wang,Libo Wang,Shihao Cui,Dejian Xu,Hui Wang,Honghao Liu,Haipeng Zhang,Ning Gong,Qingshan Zhao,Mingbo Wu
Pd-based catalysts play a pivotal role in nitroaromatic hydrogenation for fine chemical synthesis, yet their intrinsic overactivity often undermines target selectivity. In this study, we develop a highly efficient and magnetically recoverable Pd/Fe3O4–rGO catalyst for nitroaromatic hydrogenation through dual-support interfacial engineering, realized by precisely anchoring Pd nanoparticles at the heterojunctions of ferrosoferric oxide and reduced graphene oxide (Fe3O4–rGO). The dual-support modulation effect not only ensures uniform Pd distribution via strong interfacial interaction but also drives directional charge transfer from Pd to the Fe3O4–rGO composite support, synergistically enhancing nitro group adsorption and optimizing H2 dissociation kinetics. The prepared Pd/Fe3O4–rGO catalyst achieves exceptional catalytic performance with 99% conversion and >97% selectivity for the chemoselective hydrogenation of diverse nitroaromatics under mild conditions while maintaining remarkable activity/selectivity over multiple cycles. Notably, the integrated Fe3O4 component facilitates efficient magnetic separation (<2 min), demonstrating industrial viability for continuous processes. This work provides a rational dual-support strategy that simultaneously regulates spatial configuration and electronic states of active sites to overcome the activity-selectivity trade-off in hydrogenation catalysis.
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