JOURNAL OF CATALYSIS
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2026
·
IF 6
De Xia,Hao Wang,Ben Li,Bing Lu,Yong Wang,Shanjun Mao
This study presents a novel Rh 7 Ni 1 P 4 /SiO 2 catalyst that significantly improves the hydroformylation of olefins, achieving a turnover frequency of 3433h −1 . By incorporating nickel (Ni) and phosphorus (P) into rhodium (Rh), the electronic structure of Rh was effectively modified, enhancing olefin adsorption and reducing CO binding energy. This dual modulation boosts catalytic performance by shifting the rate-determining step from CO insertion to acyl hydrogenation, thereby accelerating the reaction rate. Experimental results, supported by density functional theory (DFT) calculations, reveal that the Rh 7 Ni 1 P 4 /SiO 2 catalyst reduces Rh-CO interactions, minimizes rhodium leaching, and exhibits excellent stability over multiple cycles. This research advances the design of robust and efficient catalysts for industrial hydroformylation processes.
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高影响因子
ACS Applied Materials & Interfaces
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2026
·
IF 7.8
Feng Han,Zhen Ye,Shaoze Wang,Wenfeng Shangguan,Zhi Jiang
Facet engineering is an effective strategy for enhancing the photocatalytic performance of semiconductor single crystals. However, conventional high-temperature solid-state synthesis often suffers from coupled crystallization and grain coarsening, making it difficult to simultaneously achieve high crystallinity, controlled facet exposure, small particle size, and good dispersibility. Herein, we report an integrated strategy combining solid-state recrystallization and facet engineering for the synthesis of small-sized SrTiO3:Rh single crystals with co-exposed (100)/(110) facets. Specifically, this approach employs partially crystallized SrTiO3 nanosphere precursors, which are subsequently subjected to SrCl2 molten-salt-assisted high-temperature recrystallization to enable crystal reconstruction, while suppressing excessive grain growth. The incorporation of Rh, together with the SrCl2 molten-salt environment, influences crystal growth behavior and facilitates selective facet exposure, which is associated with the formation of octadecahedral SrTiO3:Rh single crystals. The resulting particles simultaneously exhibit high crystallinity, anisotropic facet exposure, reduced particle size, and enhanced suspension stability in aqueous media. These structural features are closely correlated with improved charge carrier separation behavior and higher mass-normalized activity under low catalyst loading conditions. Compared with conventional Rh2O3-derived SrTiO3:Rh, the optimized samples exhibit significantly enhanced charge separation behavior and photocatalytic hydrogen evolution performance. Furthermore, upon Cr co-doping, the SrTiO3:Rh,Cr/BiVO4 system with the highest activity among the investigated Cr concentrations, coupled with the Fe3+/Fe2+ redox mediator, achieves an apparent quantum yield (AQY) of 4% under 420 nm monochromatic irradiation and demonstrates stable overall water splitting activity in a liquid-phase Z-scheme configuration.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Zenghao Shi,Zhou Ren,Wenqiang Yang,Jingwei Li,Yang Zhao,Wenhao Cui,Feifei Xu,Shuwen Yu,Dehui Deng,Li Yan,Yunjie Ding
Ni/Rh nanoalloy matches the rates of two sub-reactions for urea electrosynthesis. • Rh-driven *CO dispatching redirects the reaction pathway from CO to urea. • Comprehensive in situ ATR-SEIRAS elucidates the distinct roles of Ni and Rh. • The FE Urea /FE CO for Ni/Rh nanoalloy boosts 30 times than that of Ni-BNC. The electrocatalytic co-reduction of CO 2 and nitrate (NO 3 - ) presents a sustainable route for urea synthesis, yet it is severely hampered by mismatched activation rates of the two sub-reactions (CO 2 reduction reaction and nitrate reduction reaction). Herein, building on our previous study of Ni-BNC for CO 2 to CO conversion, we constructed a Ni/Rh nanoalloy catalyst (Ni/Rh-BNC) via Rh-incorporation strategy to effectively redirect reaction pathway to urea from CO. Systematic in situ ATR-SEIRAS and Raman spectroscopy provide mechanistic insights into the intermediate evolution and reaction pathway switching. While Ni acts as a *CO generator, the incorporated Rh species serves a triple regulatory role: (i) activating NO 3 - to balance the two sub-reaction rates; (ii) stabilizing *CO intermediates generated from adjacent Ni sites via *CO transfer; and (iii) directly initiating C-N coupling to form urea. This Rh-driven *CO “dispatching” mechanism suppresses CO desorption and steers the pathway toward urea formation. Consequently, the urea-to-CO Faradaic efficiency (FE) ratio for Ni/Rh-BNC boosts nearly 30 times than that of Ni-BNC, achieving a urea FE of 31.2% at −0.7 V vs. RHE, with a maximum urea yield of 7981.8 mg·g metal −1 ·h −1 under low metal loading conditions. This strategy underscores a promising blueprint for rational catalyst design of dual metal sites enabling reaction pathway redirection and sub-reaction rate matching for multi-step electrocatalytic reactions. Download: Download high-res image (195KB) Download: Download full-size image
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ACS Sensors
·
2026
·
IF 10.9
Xiong Haichao,Xu Shusheng,Wang Tao,Ni Wangze,Wang Zhaozhao,Chen Yiting,Shi Xuerong,Zhao Lipeng,Li Ming
High-performance hydrogen (H 2 ) sensors are essential for industrial safety and environmental monitoring. Herein, we report a microelectromechanical system (MEMS) H 2 sensor based on SnO 2 nanoflowers in situ decorated with PdRh nanoparticles (PdRh/SnO 2 ). Gas-sensing evaluations demonstrate that the sensor exhibits an ultrahigh response ( R a / R g ) of 20.2 to 100 ppm H 2 , representing a nearly 4-fold enhancement compared to the conventional Pd/SnO 2 sensor. Furthermore, it displays rapid response and recovery times of merely 1.7 and 2.2 s, equivalent to ∼63 and ∼34% of those exhibited by the Pd/SnO 2 counterpart, respectively. Additionally, the device achieves a notably low detection limit below 100 ppb alongside good long-term stability. Mechanistic studies combining experiments and density functional theory (DFT) calculations reveal that this significant performance enhancement originates from a dual mechanism. While the synergistic catalytic dissociation of H 2 by the PdRh nanoalloy contributes to the improved sensing kinetics, we uncover a more critical role of Rh: it lowers the desorption energy barrier of lattice oxygen in SnO 2 , thereby inducing the formation of high-density oxygen vacancies at the heterointerface. This Rh-mediated defect engineering promotes the adsorption and generation of reactive oxygen species, providing abundant active sites for H 2 reactions and substantially amplifying the sensing response. Finally, the PdRh/SnO 2 -based MEMS sensor was successfully integrated into a portable wireless monitoring system, validating its tremendous potential for H 2 detection applications.
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PubMed
高影响因子
Catalysts
·
2025
·Vol. 15
·期 12
·1122
·
IF 4
Yuting Dai,Xuemin Cao,Fei Qian,Xia Li,Li Zhang,Peng He,Zhi Cao,Chang Song
The direct synthesis of long-chain α-olefins from syngas offers a strategically vital pathway for producing high-value chemicals from alternative carbon resources. However, achieving high selectivity toward C5+olefins remains challenging due to competing paraffin formation and difficulties in precisely regulating chain growth kinetics. To mitigate these critical challenges, a series of Rh-promoted Co-Mn catalysts supported on SiO2were synthesized using a carbon-mediated impregnation strategy for the direct conversion of syngas to long-chain α-olefins (C5+). The introduction of Rh significantly enhanced both catalytic activity and C5+olefin selectivity. The optimal 1.1 wt% Rh-loaded catalyst achieved 24.6% CO conversion and 46.0% total olefin selectivity, with 34.2% of the selectivity toward C5+olefins, while maintaining low CH4(6.2%) and CO2(<1%) selectivity. Comprehensive characterization techniques, including XRD, H2-TPR, XPS, and TEM/HAADF-STEM, revealed that the carbon-mediated method facilitated the formation of highly dispersed Co3O4nanoparticles with abundant oxygen vacancies and strengthened the Co-MnOxinterface. Rh promotion modulated the cobalt speciation (Co0/Co2+), improved reducibility, and enhanced the metal-support interaction. This promoted chain growth and olefin desorption while suppressing over-hydrogenation. This study demonstrates the efficacy of Rh promotion and carbon mediation in designing high-performance Fischer-Tropsch catalysts for selective α-olefin synthesis, offering new insights into the design of efficient metal-oxide interfacial catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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能源与燃料
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无机化学
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Chemistry-An Asian Journal
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2024
·Vol. 19
·期 14
·e202400342
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IF 3.5
Yuanxin Cao,Xiaoming Yu,Tianfu Wang,Jiahao Li,Nan Li,Anbang Ge,Jie Ying,Tongwen Yu
Here, we report the systematical synthesis of zeolite-templated carbon (ZTC) supported Ru and Rh mono- or bi-metallic electrocatalysts towards hydrogen evolution reaction (HER). The zeolite A or ZSM-5 derived ZTC supports and metal sites were adjusted, and all electrocatalysts outperformed the commercial Pt/C electrocatalyst for HER performance. In particular, the RhRu/(ZTC/ZSM5) sample exhibited superior catalytic performance with the overpotential of 24.8 mV@10 mA ⋅ cm −2 , and outstanding stability with 1 mV drop after 20000 cyclic voltammetry circles. This work offers a simple impregnation method for the synthesis of highly performed HER electrocatalysts supported on porous zeolite-templated carbon.
研究领域:
材料科学
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电化学
·
催化
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PubMed
高影响因子
CATALYSIS TODAY
·
2019
·
IF 4.888
Huixian Zhong,Jiaming Wang,Kang An,Jie Yang,Zhi Ma,Hong Wang,Yuan Liu
A new catalyst for direct ethanol synthesis (DES) from syngas composed of Rh nanoparticles (NPs) highly dispersed on La-Ce-O modified LaFeO 3 which was loaded on SiO 2 support was studied in this work. Over the best catalyst 40.6 % of the reacted CO could be directly converted into ethanol with CO conversion of 14.2 % at 250 °C, 3 MPa and GHSV of 3900 mL (g cat h) −1 . The results indicated that adding cerium into LaFe 0.5 Rh 0.5 O 3 /SiO 2 resulted in La 1-x Ce x Fe 0.5 Rh 0.5 O 3 /SiO 2 , the incorporation of Ce effectively regulated the interface electronic states of Rh NPs . The well matched catalyzing process by the active sites of Rh 0 , Rh + (or Rh δ+ ) and the oxygen vacancies on the surface of LaFeO 3 , of those, Rh 0 dissociatively adsorbed CO and the latter two associatively adsorbed CO could effectively improve the activity and selectivity for DES. Moreover, the interaction of La-Ce-O and LaFeO 3 strengthened the CO adsorption on the oxygen vacancies on LaFeO 3 , which improved the capacity of assistance in activating CO associatively, thus further increasing the selectivity to ethanol. The catalyst exhibited excellent resistance to carbon deposition and sintering, attributing to the small size of Rh NPs and the carbon eliminating effect of La 2 O 3 and oxygen vacancies on the surface of LaFeO 3 .
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ACS Applied Energy Materials
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2026
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IF 5.5
Yanan Li,Minjie Wang,Jiaqi Shao,Huajie Huang,Xinggang Shan,Haiyan He
Direct methanol fuel cells have attracted extensive research interest, yet their practical advancement remains constrained by the inadequate activity and durability of conventional platinum-based anode catalysts. In response to these limitations, here we develop a non-platinum catalyst consisting of ultrafine rhodium nanocrystals confined within a ruthenium dioxide-modified hollow carbon sphere (Rh/RuO2−HCS) through a stepwise stereoconstruction approach. The hollow carbon sphere framework with plentiful mesoporous channels facilitates the transport of both electrons and ions, while RuO2 acts as a co-catalyst that supplies abundant hydroxyl species to oxidize CO intermediates, both of which are conducive to fully realizing the catalytic functions of Rh component. Benefiting from this synergistic design, the optimized Rh/RuO2−HCS catalyst exhibits outstanding methanol electrooxidation performance with large electrochemical surface area, high mass activity, and reliable durability, significantly superior to unmodified HCS and conventional carbon black-supported Rh catalysts.
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Materials Today Energy
·
2021
·
IF 7.311
H. Yu,Z. Wang,W. Tian,Z. Dai,Y. Xu,X. Li,L. Wang,H. Wang
Electrochemical nitrogen reduction reaction (NRR) has been regarded as one of the most promising alternative strategies for nitrogen fixation, and the design of efficient NRR catalysts is the critical factor. Herein, boron and sulfur co-doped mesoporous Rh film on Ni foam (B, S-mRh/NF) is developed for electrochemical ammonia synthesis. The boron and sulfur co-doping, the B, S-mRh/NF, can inhibit competitive hydrogen evolution reaction effectively. Owing to binder-free mesoporous structures, binder-free characteristic, and multicomponent alloy, the B, S-mRh/NF displays a high NH 3 yield of 11.88 μg/h/cm 2 at −0.1 V and Faraday efficiency of 38.42% at −0.05 V in neutral electrolyte. This work offers an effective strategy for the rational design of nonmetal-doped porous Rh electrocatalysts with self-supported structure, which would be highly potential for the electrochemical ammonia synthesis.
研究领域:
化学工程
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材料科学
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电化学
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高影响因子
PHOTOCHEMISTRY AND PHOTOBIOLOGY
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2025
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IF 2.5
Yao Zhang,Shiming Zhang,Li Luo,Sansan Hu,Xujuan Huang,Yongzheng Chen
Using visible light to drive NADH regeneration is an economically viable and environmentally sustainable technique. However, it necessitates a metal hydride (MH, [CpRh(bpy)(H 2 O)] 2+ ) as a synergist, and the high cost of the Rh noble metal significantly impedes the development and application of in-situ NADH regeneration. Therefore, in this study, single-atom Rh was immobilized onto the CdS QDs@SiO 2 combination via a consecutive ball-milling technique in combination with ionic layer adsorption and substitution. Subsequently, an enhanced photo-metal synergistic catalysis system for the recyclable regeneration of NADH was developed. In this composite, the single-atom Rh serves two main functions: It acts as an electrical medium and a metal catalyst, which regulates the activity and selectivity of the regenerated NADH. This study has successfully addressed the key scientific issues regarding the low electron transport rate and the recycling of the Rh noble metal during catalysis. Results confirm that single-atom Rh is successfully immobilized onto the CdS QDs@SiO 2 combination (Rh-CdS@SiO 2 ) and exhibits a faster electron transport and enhanced selectivity. Under blue light (LED, 420 nm) irradiation, the Rh-CdS@SiO 2 photo-metal catalyst shows a 25-fold increase in recyclable operability and achieves a 68% regeneration yield of NADH in just 4 min. Moreover, (S)-(+)-4-phenyl-2-butanol can be obtained with the regenerated NADH as the coenzyme of P450 enzyme catalysis.
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ACS Catalysis
·
2021
·
IF 13.084
Boyang Liu,Ning Huang,Yu Wang,Xiaocheng Lan,Tiefeng Wang
Rh-based homogeneous catalysts with phosphine ligands are highly active in hydroformylation reactions. Using DFT calculations, we found a similar electronic effect of inorganic phosphorus in the Rh2P structure. The energy profiles demonstrated that Rh2P would significantly enhance the styrene hydroformylation activity in comparison with Rh, which was further confirmed by experiments. Triphenylphosphine (PPh3) was used as the phosphorus source, and Rh2P supported on silica was prepared by impregnation at a relatively low temperature (550 °C). The turnover frequency (TOF) of styrene hydroformylation was increased to 1496 h–1, which was comparable with some single atom catalysts (SACs). Recycling tests showed a good stability in five runs. Furthermore, HAADF-STEM, XPS, and other characterizations confirmed the synthesis of the Rh2P structure. The promotion effect of P was bifunctional. On the one hand, the doped P separated the surface Rh atoms, which eliminated the surface hollow sites and prevented excessively strong adsorption of the reactants. On the other hand, electrons transferred from Rh to P, causing the surface Rh atoms to be positively charged, which was favorable for hydroformylation reactions. The geometric effects improved the dispersion and the electronic effects changed the rate-determining step from CO insertion to phenylpropionyl hydrogenation, both leading to a higher hydroformylation activity.
研究领域:
化学
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材料科学
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Catalysts
·
2022
·Vol. 12
·期 1
·83
·
IF 4.501
Cuiping Yu,Weilong Wu,Min Gao,Yu Liu
Asymmetric catalysis is the preferred method for the synthesis of pure chiral molecules in the fine chemical industry. Cellulose has long been sought as a support in enantioselective catalysis. Dialdehyde cellulose (DAC) is produced by the selective oxidation of cellulose and is used to bind 5,5′-diamino Binap by forming a Schiff base. Here, we report the synthesis of modified cellulose-supported Rh as a novel biomass-supported catalyst and the characterization of its morphology, composition, and thermal stability. DAC-BINAP-Rh was a very effective catalyst in the asymmetric hydrogenation of enamides and could be easily recycled. This work provides a novel supported catalyst that broadens the applications of cellulose in asymmetric catalysis.Keywords:asymmetric hydrogenation;cellulose;BINAP;heterogeneous catalysis
研究领域:
化学
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材料科学
·
有机合成
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高影响因子
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