Journal of the American Chemical Society
·
2025
·
IF 15.6
Qipei Sun,Shiya Chen,Xuan Huang,Xia Lv,Yang Sun,Tingjie Mao,Juan Wang,Tingshan Chan,Yu-Cheng Huang,Zhiwei Hu,Qi Shao,Xiaoqing Huang
Phase engineering is a significant means of effectively enhancing catalytic performance. However, achieving continuous and precise phase control in intermetallic compounds remains a challenge, which has hindered the development of phase-dependent catalysis. In this work, we demonstrate continuous phase regulation and unveil the crucial role of phase rearrangement in the selective construction of nanocrystals. Through a mechanistic investigation, we uncovered a phase-dependent behavior governing the selective phase transformation during phase rearrangement. When a Pd-rich (Pd20Te7, the ratios of Pd/Te > 1) template was used, Pd20Te7 rearranged into PdTe. The Te vacancies generated in this process were occupied by Pb atoms, leading to the formation of a Pd–Pb alloy. Conversely, Te-rich template (PdTe2, the ratios of Pd/Te < 1) rearranged to PdTe, with the resulting Pd vacancies being occupied by Pb atoms to form a Pb–Te alloy. The customized interface in PdTe–PbTe significantly enhanced its formic acid oxidation reaction (FAOR) activity. The catalyst achieved a mass activity of 4.17 A mgPd–1 and a specific activity of 9.12 mA cm–2, surpassing commercial Pd/C by factors of 16.68 and 12.67, respectively. This work establishes a selective phase-regulation strategy to create customized nanostructures for diverse applications.
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Molecular Catalysis
·
2026
·
IF 4.3
Shukang Ti,Dongmei Yue
Pd/DUT-5 is an efficient catalyst for NBR hydrogenation to HNBR. • High hydrogenation activity was achieved under mild conditions. • Metal-support interactions stabilize electron-enriched Pd δ+ species. • Pd δ+ species enhance catalytic activity and chemoselectivity. • DFT reveals low-barrier heterolytic H 2 activation at Pd δ+ –μ 2 O - sites. Hydrogenated nitrile butadiene rubber (HNBR), produced via the selective hydrogenation of nitrile butadiene rubber (NBR), has attracted considerable interest because of its excellent overall performance. However, the development of efficient and selective catalytic systems for NBR hydrogenation under mild conditions remains challenging, particularly when both activity and cost-effectiveness are required. Herein, Pd nanoparticles were immobilized on the Al-based metal-organic framework DUT-5, and the influences of Pd precursor salts and pretreatment conditions on catalytic hydrogenation performance were systematically investigated. The results show that using Pd(OAc) 2 as the precursor in combination with relatively low reduction temperatures promotes the formation and stabilization of electron-enriched Pd δ+ species through metal-support interactions, leading to excellent low-temperature activity and good reusability, with the hydrogenation degree remaining 94.5% after three cycles. Density functional theory calculations using C 2 H 4 as a model substrate further reveal that Pd δ+ sites cooperatively interact with μ 2 O - moieties to facilitate H 2 activation and subsequent hydrogen transfer through a heterolytic cleavage pathway with reduced energy barriers. These results provide a mechanistic basis for the efficient hydrogenation of NBR under mild conditions. Overall, this work demonstrates an effective and economical strategy for HNBR production and offers new insights into the design of highly active and chemoselective catalysts for NBR hydrogenation. Download: Download high-res image (205KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Lan Zhang,Wanran Huang,Xi Peng,Peixin Jiang,Jianshan Ye,Minglei Yan,Zhiwei Lu
The high efficiency, low cost, and rapid preparation of non-noble metal oxygen reduction reaction (ORR) electrocatalysts are of great significance for the large-scale application of energy conversion equipment. Herein, PdNi alloy nanoparticles dispersed within the multiwalled carbon nanotubes (MWCNTs) composite (PdNi-PVP/MWCNTs) were synthesized via an in situ self-assembly strategy, in which polyvinylpyrrolidone (PVP) serves as an N and C source, and MWCNTs act as conducting supports to enhance structural integrity and electron transport. Notably, the synthesis relies solely on low-temperature oil-bath stirring, enabling rapid batch production without the need for high-temperature calcination-a distinctly green and scalable approach. In this system, PVP acts as a capping agent that facilitates the uniform anchoring of PdNi alloy nanoparticles on MWCNTs, effectively suppressing particle aggregation, thereby increasing the surface roughness and specific surface area to expose more active sites. Impressively, benefiting from the unique structure, high crosslinking, and high conductivity that minimize catalyst separation and aggregation, this new type of electrocatalyst exhibited an impressive ORR onset potential of 0.97 V, half-wave potential of 0.83 V, larger current density of 4.3 mA∙cm −2 , and existing good corrosion resistance to drive a relatively stable performance, which are superior to commercial Pt/C in alkaline media. This study demonstrates the successful design of an environmentally benign and cost-effective ORR electrocatalyst, highlighting its promising potential for practical applications in energy conversion technologies.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2026
·
IF 6.7
Yiran Sun,Xingyue Zhou,Sikai Dai,Yu Fan,Chengkun Xie,Ruoqi Wang,Jun Qian,Lingzhi Nie,Peiyuan Zuo,Qixin Zhuang
High-entropy alloys (HEAs) are promising electromagnetic absorbers owing to tunable magneto-dielectric properties, yet severe particle agglomeration and grain coarsening severely degrade their wave-absorbing capacity. Herein, a Pd-mellitic acid ligand-induced strategy is developed to immobilize uniform FeCoNiCuPd quinary HEA nanoparticles on one-dimensional hollow mesoporous carbon nanorods (CPMO@5 A). Multidentate carboxyl groups of mellitic acid serve as universal coordination sites for synchronous multi-metal nucleation, effectively restraining HEA aggregation and triggering prominent grain refinement and lattice distortion driven by high configurational entropy. Benefiting from hierarchical porous architecture, uniform-dispersed HEA nanoparticles and abundant heterogeneous crystal defects, CPMO@5 A achieves superior electromagnetic wave absorption. It delivers a minimum reflection loss of −76.6 dB at 2.7 mm and an ultra-wide effective absorption bandwidth of 8.4 GHz, covering the entire Ku-band and most X-band. Meanwhile, it exhibits infrared absorptivities of 98.2%, 98.9% and 97.7% in long-wave, mid-wave and short-wave infrared regions, outperforming most reported HEA absorbers. Dielectric loss from Cu and carbon matrix, coupled with magnetic loss of Fe, Co, Ni and Pd, synergistically promotes electromagnetic energy dissipation. This work provides a facile universal route for fabricating HEA-based electromagnetic materials for high-performance radar-infrared compatible stealth materials.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2026
·Vol. 40
·期 4
·e70553
·
IF 4.3
Lichun Xu,Jianbo Li,Wenbo Ma,Tianzhu Yin,Mengbi Guo,Rui Yang,Bo Yang
Transition metal-catalyzed C-C couplings have the potential to provide complex molecules, however, the formation of selective C–C bonds for symmetric/unsymmetric dihalogenated aromatics remains being a challenge. To explore the specificially selective Suzuki monocoupling of symmetrical/unsymmetrical dibromopyridines, a set of cross-linked cyclodextrin polymers ( CD-P ) were synthesized by CuAAC reaction and coordinated with Pd ( CD-P-Pd (II) ). Numerous cavities with pocket-like catalytic sites were designed in its structure and the narrow rims of cyclodextrin were connected and enclosed by triazole rings coordinated with Pd. Meanwhile, the wide rims were kept open to recognize the reactants and products for association and dissociation with the cavity. The use of CD-3-P-Pd (II) under mild conditions can obtain monosubstituted products with yield of up to 79% and specific selectivity (mono−/bis- = 100:0 for symmetrical dibromopyridines, monoaty−/monoty−/bis- = 80:0:20 for unsymmetrical dibromopyridines). This mechanism study supports the hypothesis that the first oxidation addition step can be effectively regulated by the structural design of the catalyst to obtain monosubstituted products. Cyclodextrin polymers offered exciting possibilities for the specificity of coupling reactions by facilitating host-guest recognition.
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Nature Communications
·
2026
·
IF 18.1
Hong Feng,Chen Hongqiu,Chen Jiawei,Ying Zhehan,Peng Mi,Zhang Jingwang,Yang Zuodong,Wen Guodong,Diao Jiangyong,Sun Bo,Sun Geng,Ma Ding,Liu Hongyang
Acetylene semihydrogenation is a critical process in the polyolefin industry by selectively removing trace acetylene from ethylene-rich reformate. However, this reaction is generally limited by the inherent activity-selectivity trade-off due to the thermodynamic advantage of overhydrogenation. Herein, we develop a facile and straightforward strategy to construct Pd 2 dual-atom sites anchored on defect-rich surface-graphitized nanodiamond (ND@G) via the solvent-mediated dispersion of palladium carboxylate driven by the chelation of palladium precursors via carboxylate anion. Cs-corrected HAADF-STEM images coupled with XAS analysis unambiguously manifest the successful architecting of Pd 2 dual-atom sites. Compared to Pd 1 single-atom sites, the obtained Pd 2 /ND@G sample demonstrates superior catalytic performance in acetylene semihydrogenation, with the corresponding TOF values increased from 0.151 s −1 to 1.953 s −1 , without the obvious decline of ethylene selectivity (93.2%, at full acetylene conversion). C 2 H 2 /C 2 H 4 -TPD, H 2 -D 2 exchange reaction, isotope-labeled TPSR combined with DFT calculations confirm the effective co-activation of C 2 H 2 /H 2 on Pd 2 dual-atom sites while maintaining the weak adsorption of ethylene similar to that on its single-atom sites, which can break the activity-selectivity trade-off in acetylene semihydrogenation.
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ACS Sensors
·
2026
·
IF 10.9
He-Jie Wang,Hao-Nan Chen,Xuan-Yu Yang,Fei-Long Gong,Ke-Feng Xie,Shi-Zhong Wei,Yong-Hui Zhang
The development of highly sensitive and reliable hydrogen detection technology is a critical prerequisite for the safe and large-scale application of green hydrogen energy. Pd-based metal oxide semiconductor sensors exhibit decent sensing performance; however, their development for hydrogen detection is hindered by competitive adsorption of hydrogen and oxygen on the surface and sluggish reaction kinetics due to limited active interfaces. Here, a series of Pd nanoparticle-decorated, K+ interstitial doping WO3 nanosheets (PdNP-K/WO3-x) were synthesized. The optimized PdNP-K/WO3-15 sample exhibited exceptional H2 sensing performance, including a high response (Ra/Rg = 1235.94 to 50 ppm H2) at a low temperature of 130 °C, with fast response/recovery. This enhancement stems from synergistic effects where K+ interstitial doping increases electron density and oxygen vacancies in WO3, improving charge transfer and strengthening the W-O-Pd interface. The resulting electron-rich environment also shifts the d-band center of Pd, enhancing hydrogen desorption and spillover, while reducing competitive oxygen adsorption to free up more Pd active sites. The material also showed promising room-temperature sensing, indicating strong application potential and providing a theoretical basis for designing high-performance alkali metal ion-doped metal oxide materials.
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Aggregate
·
2026
·Vol. 7
·期 3
·e70308
·
IF 14.5
Hao Liu,Lingwen Liao,Wanmiao Gu,Runguo Wang,Qing You,Zhen He,Zongbing He,Zhiyuan Lin,Zhikun Wu
Although metal nanoclusters (NCs) are ideal building units, significant challenges remain in manipulating their gathering and tuning the as-obtained aggregate properties. Herein, we introduce an electro-driven strategy and reveal the voltage-dependent assembly on interdigitated microelectrodes based on Au 25 NCs: crystallizing at 0.5 V, NC-based filming at 1.3 V, and nanocrystal-based filming at 2.6 V. More interestingly, the film formed at 2.6 V can be varied from an insulator to a conductor, and even such a large conductivity tunability (from ∞ to ∼0.3 Ω) can be extended to the films formed from some other metal NCs such as Ag 25 , Pt 23 , and Pd 8 . The as-obtained films show novel, promising properties not found in molecular NCs, as illustrated by the electrothermy and current-limiting properties. Thus, this work not only provides a novel strategy for metal NCs’ gathering but also pioneers metal NC-based electro-manufacturing for novel findings and potential applications.
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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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ACS Catalysis
·
2025
·
IF 13.1
Xinrui Shi,Guoju Yang,Min Zhang,Xiangyu Liu,Wei Zhang,Yue Liu
Aqueous pH modulates the transition-metal-catalyzed hydrogenation reaction, enhancing the rate in the presence of high concentrations of hydronium ions (H3O+) to the metal. Herein, Pd particles encapsulated in hydrophobic silicalite-1 zeolite pores (Pd/S1-in) were synthesized and tested for benzaldehyde hydrogenation in water. Hydrophobic silicatlite-1 excludes the retention of both H2O and H3O+ within its pores, preventing the direct proximity of H3O+ to Pd particles. However, the hydrogenation rate of benzaldehyde on Pd/S1-in showed a pronounced dependence on the aqueous pH, with the rate increased by one order of magnitude as the pH decreased from 9 to 4. We propose that silanol groups (SiOH) of silicatlite-1 dissociate in water, forming an acid/conjugate base pair of SiOH/SiO–. This pair creates an acidic environment within the silicalite-1 pores that mirrors the pH of the bulk aqueous solution, enhancing the hydrogenation activity of the encapsulated Pd particles and demonstrating an indirect yet substantial influence of bulk solution pH on the catalytic performance of Pd/S1-in.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 2
·121185
·
IF 7.2
Peng Gao,Li Liu,Guirong Bao,Dequan Chen,Jia Luo,Xuewu Ji,Wenyao Deng
The conversion of furfural (FF) to cyclopentanone (CPO) via selective hydrogenation-rearrangement represents a crucial route for sustainable, high-value valorization of renewable biomass feedstocks. In this study, carbon dots (CDs) were utilized as both a reducing and a dispersing agent for the one-pot green photoreduction synthesis of PdAg bimetallic catalysts supported on CDs (Pd x Ag y /CDs) in aqueous phase. Among the catalysts with varying Pd-to-Ag molar ratios, the Pd 0.5 Ag 1 /CDs catalyst demonstrated exceptional performance, achieving 100 % FF conversion and 93.3 % CPO selectivity within 4 h at 200 °C. The superior activity is attributed to a synergistic effect between the acid sites on the CDs and the PdAg alloy, which facilitates the rearrangement of the intermediate furfuryl alcohol (FA). Mechanistic studies, including calculations of the free energy barriers for elementary steps from FA to 4-hydroxy-2-cyclopentenone, revealed a ring-opening pathway for the furan methyl carbocation, which dramatically reduces the reaction energy barrier to 47.1 kJ/mol from 195.8 kJ/mol of the Piancatelli pathway. This work not only presents an efficient and green catalyst for FF upgrading but also highlights the promising application of CDs in advanced catalytic systems for circular economy-driven chemical production.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 16
·5490-5497
·
IF 6.4
Xiaojing Lv,Xuchen Zhu,Ling Zhang,Mi Ouyang,Minao Xia,Chunyan Liu,Cheng Zhang
Polymer-based electrochromic materials have potential application prospects in the field of displays, but the lack of a highly transparent state to red/green/blue color state limits their development and commercial applications. Herein, it is proposed to design and synthesize photo-crosslinkable polymers based on different donor or acceptor groups modified phenothiazine or triphenylamine as electrochromic units and cinnamate as photo-crosslinking units. The influences of different donor or acceptor groups, such as phenyl and methoxy, on the electrochemical and spectroelectrochemical behavior of the polymers are clarified in order to achieve neutral, highly transparent states and red/green/blue colors in the oxidation states without the intermediate color state. The crosslinkable system inside the polymer changes its intrinsic soluble characteristic into a solvent-resistant property, thus resulting in a stable polymer film via the UV irradiation method. Hence, an all-solid-state electrochromic device was fabricated by separately utilizing three photo-crosslinkable polymer films as an electrochromic layer, which shows obvious reversible electrochromism with the “RGB” patterns, demonstrating it as a candidate for electronic paper and electronic tags.
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