TETRAHEDRON
·
2024
·
IF 2.1
Zixu Li,Fei Wang,Kai Ma,Chao Fang,Qiang Jia,Changhu Chu
Aryl triflate is a type of facile and readily available compounds, which could be used as an alternative substrate for Suzuki cross coupling. In this manuscript, a novel ppm-Pd-Fe/C catalyst has been developed by reduction of palladium acetate and iron trichloride with aqueous hydrazine in situ and supported on activated charcoal. In combined with Sphos, and metal zinc as additives, this catalyst, with 300 ppm palladium loading, could be applied in the Suzuki cross coupling between aryl triflates with aryl neopentylglycolboronates.
研究领域:
有机化学
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催化
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材料科学
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高影响因子
JOURNAL OF POROUS MATERIALS
·
2020
·Vol. 28
·期 2
·487-493
·
IF 2.183
Feng Lijuan,Qiu Lu,Wang Shunli,Chang Zhaosen,Lu Yan,Dong Anwang,Chen Qi,Sui Zhuyin
The direct conversion of tremendous greenhouse gas methane into various value-added chemical products or energy fuels is not only a concern associated with an economic interest but also related to environmental protection. However, neither industry nor academia has an effective or low-cost way to directly achieve this result. Herein, a high specific area (962 m 2 g −1 ) porous organic polymer was designed and used as a substance to support catalytic active sites, including PdBr 2 , Pd(OAc) 2 , and well-dispersed AuPd bimetallic nanoparticles which were reduced via hydrogen flow. The as-synthesized catalysts (HNU-2 and HNU-3) can not only maintain the porous and stable structure of their pristine matrix but also show extremely high catalytic performance in methane direct transformation systems for preparing methanol derivative methyl trifluoroformate. Our simple strategy provides a complementary alternative to application of methane via an efficient one-step conversion procedure in order to reduce its impact on climate change and obtain value-added chemicals.
研究领域:
催化
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环境化学
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材料科学
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高影响因子
Advanced Science
·
2025
·
IF 14.1
Sisi Yao,Jiawei Han,Wenjun Zhang,Dengkang Guo,Shenjie Han,Yun Lu,Jingpeng Li
Developing efficient catalytic hydrogenation microreactors with minimal catalyst loading yet high active-site density for treating concentrated organic pollutants remains challenging. Herein, a facile room-temperature method is presented to stabilize Pd single-atom catalysts (SACs) within ZIF-67 crystals during their formation, aiming to fabricate an efficient, low-loading hydrogenation catalytic microreactor (Pd@Z-P/b CMR). ZIF-67 is constructed into polydopamine (PDA)-modified bamboo microchannels under flow conditions, utilizing preimmobilized Co 2+ seeds in PDA. Despite an ultralow Pd loading (0.0014 wt.%), the Pd@Z-P/b CMR featuring atomically dispersed Pd─N 4 sites in ZIF-67 considerably outperforms its Pd nanoparticle–loaded counterpart (Pd 0.0035 wt.%) in continuous-flow hydrogenation, demonstrating superior robustness and maximized Pd utilization with 94.3% conversion efficiency for saturated 4-nitroaniline over 10 d and 97.5% conversion efficiency for gram-level methylene blue (1.0 g L −1 ) over 5 d. Crucially, it exhibits consistent, high performance in real environmental water samples. The high surface area and porosity of ZIF-67 stabilize the Pd SACs, enhance dispersion, and ensure accessibility. Simultaneously, the Pd─N 4 configuration facilitates electron transfer and optimizes hydrogen binding energy, dramatically boosting the catalytic activity. This work provides a novel strategy for room-temperature SAC synthesis and the effective treatment of high-concentration organic pollutants for sustainable wastewater remediation.
研究领域:
环境催化
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材料科学
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纳米技术
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可持续化学
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化学工程
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DOI
PubMed
高影响因子
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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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yulu Zhang,Hangyang Feng,Weifeng Kong,Meijuan Bian,Yingying He,Qianwei Liang,Yanlong Sun,Chengzhi Zhou,Liguo Shen
A functionally graded high-entropy alloy catalyst FeCoNiCuRu 0.5 @nitrogen-doped carbon (FeCoNiCuRu 0.5 @NC) was designed to address catalytic function regulation and active-site stability challenges in peroxymonosulfate-based advanced oxidation processes. Featuring a spatially separated architecture with a Ru C composite shell and a polymetallic alloy core, the catalyst suppresses transition metal dissolution, reducing ion leaching by 65.5 % versus conventional counterparts. The catalyst achieved complete carbamazepine (CBZ) removal within 30 min with a rate constant (k) of 0.460 min −1 at pH 3, and singlet oxygen ( 1 O 2 ) and sulfate radicals (SO 4 •− ) were identified as the dominant active species. At pH 7, this rate constant (0.158 min −1 ) showed a twofold increase over that of FeCoNiCu@nitrogen-doped carbon (FeCoNiCu@NC) and a fivefold enhancement over that of Ru@ nitrogen-doped carbon (Ru@NC). The concentrations of SO 4 •− and 1 O 2 over FeCoNiCuRu 0.5 @NC are 1.97 and 3.38-fold higher, respectively, than those over FeCoNiCu@NC. This enhancement correlates with the superior charge transfer capability of the Ru-modified catalyst system. Remarkably, the FeCoNiCuRu 0.5 @NC demonstrates unprecedented pH tolerance (pH 3–11) and stability. Its dual-active-species configuration enables simultaneous degradation of electron-rich and electron-deficient pollutants, establishing a new paradigm for designing robust high-entropy alloy catalysts.
研究领域:
环境催化
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材料化学
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高级氧化过程
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污染控制化学
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纳米催化材料
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PubMed
高影响因子
Materials Science and Engineering B-Advanced Functional Solid-State Materials
·
2025
·
IF 4.6
Song Xu,Zhongxiao Zhao,Hao Jiang,Ting Chen,Ying Chen,Xianglong Zhao,Luyan Li,Bo Yang,Qiang Zhang
Direct methanol fuel cells show promise for portable electronic products, thanks to their considerable energy density and safety. However, their commercialization is hindered by challenges such as sluggish methanol oxidation reaction kinetics, high catalyst costs, and CO poisoning. This study addresses these issues by developing an oxygen vacancy-regulated MXene-supported PdSn bimetallic catalyst (PdSn/ V o -Ti 3 C 2 ) for efficient methanol oxidation reaction. The MXene support, engineered with controlled oxygen vacancies via electrodeposition, enhances electron transfer and distributes PdSn nanoparticles. The resulting PdSn/ V o -Ti 3 C 2 catalyst exhibits an outstanding electrochemical performance with mass activity of 1641 mA mg −1 , which is 3.6, 8.6, and 4.3 times as high as those of Pd/ V o -Ti 3 C 2 , Pd/Ti 3 C 2 and commercial Pd/C, respectively. Moreover, the prepared PdSn/ V o -Ti 3 C 2 catalyst also exhibits high stability. The work underscores the capability of defect engineering within MXene supports to disperse nanoparticles, which act as catalysts in direct methanol fuel cells.
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高影响因子
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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高影响因子
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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高影响因子
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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高影响因子
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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高影响因子
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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高影响因子
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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高影响因子
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