CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2026
·
IF 4
Haitao Zhou,Zhizhuo Yang,Yingping Jiang,Xiaofei Meng,Kun Huang
Liquid-liquid interfacial molecular recognition. • Water-bridged hydrogen-bonding networks as molecular sieving mechanism. • Viscoelasticity-guided molecular self-assembly for selective separation. • A novel strategy coupling interfacial states with separation performance. Controlling molecular recognition at liquid-liquid interfaces remains a formidable challenge due to the dynamic and complex nature of interfacial environments. In this study, using Dicyclohexano-18-crown-6 (DC18C6) as the molecular recognizer and sorbitan monooleate (Span80) as the viscoelastic regulator to enhance liquid film stability, a novel strategy based on viscoelastic molecular recognition is proposed, achieving controllable separation of PtCl 6 2- , PdCl 4 2- , and RhCl 6 3- . Under flow shear conditions, an ordered and dense hydrogen-bonded entangled network structure was formed at the oil-water interface by the surfactant Span80 and the macrocyclic molecule DC18C6. Spatial coordination with RhCl 6 3- anions was achieved via hydrogen-bonded water bridges interaction, through the synergistic cooperation of Span80 molecules with DC18C6 in either adjacent or opposing configurations, thereby enhancing the stability of the thin oil film. Compared to PdCl 4 2- and PtCl 6 2- , RhCl 6 3- anions exhibit a stronger hydration capacity, leading to the formation of a denser interfacial hydrogen-bonded self-assembled structure with DC18C6 and Span80 molecules. This structure can be further reinforced by adjusting the aqueous phase flow rate and the oil film thickness, thus enabling selective regulation of the differences in interfacial hydrogen‑bonding interactions. Download: Download high-res image (281KB) Download: Download full-size image
✓ 已验证
DOI
高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Jinyan Zhang,Yan Shao,Feng Zeng,Huanhao Chen
Rhodium (Rh)-based catalysts hold considerable promise for the direct hydrogenation of CO2 to ethanol (EtOH). However, their catalytic performance is often limited by high selectivity toward C1 products such as CO and CH4, a tendency largely governed by the adsorption strength of CO on Rh sites. Moderate CO interaction is hypothesized to favor the formation of lower alcohols (such as methanol and ethanol). In this work, we developed a phosphorus (P)-doped Rh/TiO2 catalyst that synergistically modulates the electronic structure of Rh and the metal−support interaction. This P-doping strategy is conducive to enhancing methanol and ethanol synthesis, particularly achieving an ethanol production rate of 1.14 gEtOH gRh−1 h−1. Moreover, the P-doped Rh/TiO2 catalyst exhibits a stable performance over 45 h on stream. Comprehensive characterizations including HAADF-STEM, XANES, XPS, and CO-DRIFTS reveal that P doping induces electron transfer from Rh to P, forming Rh2P structures that stabilize an optimized Rh+/Rh0 ratio (∼1:1) under reaction conditions. This electronic modulation weakens CO hydrogenation and promotes C−C coupling. Additionally, P doping could possibly inhibit Rh sintering and preserves the Rh2P phase, enhancing catalytic stability. In situ DRIFTS further confirmed that P doping suppresses CO hydrogenation, thereby inhibiting CH4 formation while promoting methanol and ethanol production. This work demonstrates that P-induced electronic and structural modifications offer an effective strategy for tuning CO2 hydrogenation selectivity toward lower alcohols including methanol and ethanol.
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yuanjie Xu,Zemin An,Xin Yu,Jikang Yao,Qian Lv,Hua Yang,Zhengang Lv,Huichuang Guo,Qike Jiang,Wei Liu,Lizhi Wu,Li Tan,Yihu Dai,Yu Tang
Strong metal-support interaction (SMSI) is a crucial factor that determines the structure and performance of a supported metal catalyst. Herein, the SMSI effect of Rh nanoparticle catalyst supported on h-BN is investigated in the dry reforming of methane (DRM) reactions with different CO 2 /CH 4 ratios. The catalyst characterization results demonstrate that the SMSI effect allows the Rh nanoparticles to be encapsulated by BO x overlayers under DRM reaction conditions (CO 2 /CH 4 = 1/1), which prevents the interaction between the reactants and metal centers for causing rapid deactivation. By increasing the partial pressure of CO 2 (CO 2 /CH 4 = 3/1), Rh/BN exhibits significantly enhanced activity and long-term stability in the DRM reaction. CO 2 or H 2 O in the reactive atmosphere can effectively etch the BO x overlayers for steadily exposing the active Rh-BN interface sites, as evidenced by the characterization. This observation extends the understanding of the SMSI effect at the interfaces between metal and non-oxide support.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiaolan Li,Yangqi Huang,Zhenyu Chen,Shuqi Hu,Jinliang Zhu,Panagiotis Tsiakaras,Pei Kang Shen
A series of tri-functional nanoflower (NF) catalysts with numerous nanodendrites (Pt 3 NiRh, Pt 3 NiRu, Pt 3 NiPd, Pt 3 Ni, and Pt 2 Ni 2 Rh NFs) were synthesized by introducing Rh, Ru, and Pd into Pt-Ni nanoflowers, aiming at accelerating the sluggish kinetics of oxygen reduction reaction (ORR), methanol oxidation reaction (MOR), and hydrogen evolution reaction (HER). The as-prepared catalysts displayed superior anti-poisoning ability and excellent activity due to uniform morphology and good dispersibility. Their electrochemical characterization revealed that the Pt 3 NiRh NFs showed the highest mass activity (2.17 A m g P G M - 1 ) and specific activity (3.13 mA cm -2 ) toward ORR, close to 9.9 and 4.6 times higher than the values measured on Pt/C (46.7 %). As for MOR, mass and specific activities of Pt 3 NiRh NFs were 1.88 A m g P G M - 1 and 2.62 mA cm -2 , far exceeding the values on commercial Pt/C. Moreover, HER activity of Pt 3 NiRh NFs outperformed commercial Pt/C. This work is valuable to develop promising multi-functional catalysts with enhanced activity and anti-poisoning ability.
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2022
·Vol. 18
·期 32
·2203020
·
IF 15.153
Kai Deng,Wenxin Wang,Qiqi Mao,Hongjie Yu,Ziqiang Wang,You Xu,Xiaonian Li,Hongjing Wang,Liang Wang
Tailoring the morphology and crystal structure of metallene is critical to improve its electrocatalytic performance. In this work, hetero-phase RhB metallene ( h -RhB metallene) with amorphous/crystalline structure is readily prepared by a two-step method. The h -RhB metallene is very unique in its non-metallic heteroatom doping and amorphous/crystalline structure. Benefiting from the unique metallene structure and the optimized electronic states induced by the incorporation of B atoms, the h -RhB metallene exhibits superior performance for hydrogen evolution reaction and hydrogen peroxide electro-oxidation reaction (HPOR). When coupled with HPOR, the h -RhB metallene|| h -RhB metallene water electrolysis two-electrode system exhibits a lower cell voltage of 0.379 V (@ 10 mA cm −2 ) compared with the overall water splitting (1.35 V). The presented synthetic method provides a powerful strategy to design metallene with hetero-phase for energy-saving H 2 production.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Qiangqiang Xue,Huilin Yi,Zhengwen Li,Zhao Jiang,Meng Chen,Yujun Wang,Binhang Yan,Guangsheng Luo
Surface modification of 600-µm-sized monodisperse gamma-alumina microspheres into magnesium–aluminum spinel, and co-impregnation-based loading of Rh–Ni (0.46 wt% Rh, 9.03 wt% Ni) were performed to synthesize catalysts for diesel-steam-reforming to hydrogen. The intimate interactions between Rh and Ni, the formation of the Rh–Ni alloy, and the Rh-doping-induced decrease in the particle size of Ni were determined. The DFT calculations results revealed that Rh-doped Ni(1 1 1) established remarkably weak bonds with oxygen-containing intermediates, and the reaction barrier of the rate-limiting step (CH 2 * + O* → CH 2 O*) on Rh–Ni(1 1 1) (0.76 eV) was lower than those of Ni(1 1 1) (1.14 eV) and Rh(1 1 1) (1.56 eV). The bimetallic catalyst shows the enhanced activity and resistance of sintering and carbon deposition compared with those of Ni-based (9.33 wt% Ni) and Rh-based (0.47 wt% Rh) catalysts. The catalytic performance of Rh–Ni-based catalyst was superior to that of physically mixed Ni-based and Rh-based catalysts at similar active metal loadings, which further confirmed the synergistic effect of Rh–Ni.
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·16043-16049
·
IF 3.3
Hongbo Yu,Fei Zhang,Shuibo Wang,Yang Cong,Shiwei Wang,Lin Zhu
Hydrodeoxygenation of lignin-derived phenolic compounds to produce alkanes is a promising method used for mitigating fossil energy consumption, but they often require high temperature and high pressure, resulting in their poor catalytic stability and durability. In this study, we encapsulated ∼3.9 nm active metal Rh nanoparticles (NPs) into ∼40 nm hollow mesoporous aluminosilicate nanospheres (HMANs) to synthesize M@Alx–mSiO2 nanoreactors with adjustable Al contents for guaiacol hydrodeoxygenation. The optimized Rh@Al2.0–mSiO2 catalyst displayed significantly enhanced guaiacol activity and cyclohexane selectivity relative to the Rh@mSiO2 catalyst under mild reaction conditions. According to the characterization results, the high hydrodeoxygenation activity of Rh@Al2.0–mSiO2 could be attributable to the synergistic effect between the metallic Rh and Lewis and Brønsted acid sites, and the introduction of Al species greatly facilitated the adsorption of 2-methylcyclohexanol, thereby enhancing cyclohexane selectivity. The confinement effect of Rh NPs inside the hollow cavities effectively prevents the leaching and aggregation of Rh NPs, thereby improving their catalytic durability and stability.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Xuan Zhu,Yan Liu,Menglin Wang,Li Zhang,Qiaoli Li,Entao Zhang,Hongfen Mo,Yuan Gao,Chenyu Xu,Yanwei Zhang
The synergistic coupling of light and heat in solar energy has attracted increasing research attention. In this work, both codoping and coloading were applied to SrTiO 3 -based catalysts to improve their solar photo and thermal conversion, respectively, and maximum productivities of 51.55 and 25.59 mmol·g −1 ·h −1 were achieved for H 2 and O 2 in photothermal synergistic water splitting. The yield of H 2 was nearly double that achieved via pure photocatalysis. In addition to many experiments and characterizations, DFT calculations were also performed to clarify the photothermal synergy. It was found that both the light absorbance and mobility of photoinduced carriers could be promoted by solar thermal effects in the material. Meanwhile, the energy barriers of the key steps were reduced with increasing temperature in the hydrogen production driven by solar photo effects. This work offers new ideas for designing catalysts for solar hydrogen production with photothermal synergistic strategies.
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Lihua Zhu,Huaze Zhu,Mohsen Shakouri,Linghai Zeng,Zhiqing Yang,Yongfeng Hu,Hengqiang Ye,Hui Wang,Bing Hui Chen,Rafael Luque
Mono- and bimetallic nanoparticles (NPs) supported on carbon nanotubes (CNTs) (Ni/CNTs, Co/CNTs and NiCo/CNTs) were synthesized at room temperature (RT) via hydrazine hydrate reduction method without any surfactant. The galvanic replacement reaction was exploited to prepare Rh/Ni/CNTs, Rh/Co/CNTs and Rh/NiCo/CNTs supported nanocatalysts. Prepared nanocatalysts were extensively characterized using an array of advanced analytical techniques. The catalytic performance of the catalysts was evaluated in the hydrogenation of tetralin. Reduced Rh/NiCo/CNTs catalyst (Rh-on-NiCo NP) exhibited high catalytic activity at RT, significantly improved as compared to Rh/Ni/CNTs and Rh/Co/CNTs due to the interfacial nano-synergy effect among different metallic related species (Rh, Ni and Co). In-situ XAS results confirmed the mechanism of the interfacial nano-synergy effect, wherein Rh sites provided activated hydrogen species (H*), and H* was subsequently transferred to the surface of NiCo NPs; while tetralin was adsorbed and activated at NiCo sites, reacting with H* to produce decalin. The present work proposed a novel strategy to design highly efficient and stable multimetallic catalysts for heterogeneous catalytic hydrogenation reactions.
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Qiqi Mao,Shiqian Jiao,Kaili Ren,Shengqi Wang,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang
Rhodium (Rh) -based nanomaterials are promising alternatives to platinum (Pt) for the hydrogen evolution reaction (HER). However, the engineering and synthesis of Rh-based electrocatalysts to achieve Platinum-like HER performance under a comprehensive pH range still remains a challenge. In this work, we report an effective tactics to promote the HER performance of Rh mesoporous nanoparticles (Rh MNs) by co-doping of transition metal (e.g., Ni, Co, Fe) and phosphorus (P) elements. Such a metal-nonmetal co-doping could effectively regulate the electronic structure, increase the active sites, and induce lattice strain, which jointly contributes to a superior HER performance. With these merits, the optimized RhNiP mesoporous nanoparticles (RhNiP MNs) exhibited superior HER activity in a comprehensive pH scope, requiring overpotentials of only 15 mV, 36 mV and 44 mV in 0.5 M H 2 SO 4 , 1 M KOH and 1 M phosphate buffer solution (PBS), respectively, at the cathodic current density for 10 mA cm −2 .
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Nan Jia,Yanping Liu,Lei Wang,Pei Chen,Xinbing Chen,Zhongwei An,Yu Chen
The development of highly effective and low-cost electrocatalysts for energy-saving hydrogen production via water splitting is still a great challenge. Herein, porous nitrogen-doped carbon nanobowls (N-CBs) have been designed and used for the controlled growth of ultrafine rhodium (Rh) nanoparticles. With the aid of interfacial bonding of Rh and N, ultrafine Rh nanoparticles with an average size of 1.4 nm have been successfully immobilized on the N-CBs. This Rh/N-CB electrocatalyst shows superior activity and high stability for the hydrogen evolution reaction (HER) and the hydrazine oxidation reaction (HzOR). More importantly, the Rh/N-CBs exhibit high activity for hydrogen production from water electrolysis, marking with a cell voltage of 0.2 V to achieve a current density of 20 mA cm–2 when they serve as cathodic electrocatalysts for the HER and anodic electrocatalysts for the HzOR in 1 M KOH with 0.5 M hydrazine. The density functional theory calculations demonstrate that a near-zero hydrogen adsorption free energy produced by the chemical bonding of Rh with the pyrrole-N doped in N-CBs is responsible for the excellent HER activity of Rh/N-CBs electrocatalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
HYDROMETALLURGY
·
2019
·
IF 3.465
Shunyan Ning,Shichang Zhang,Wei Zhang,Jie Zhou,Siyi Wang,Xinpeng Wang,Yuezhou Wei
The separation of fission products Ru, Rh, and Pd will benefit both the nuclear fuel cycle and enlarge the platinum group metals source. A silica-based iso Bu-BTP/SiO 2 -P adsorbent was used to separate Ru, Rh, and Pd from nitrate solution. It exhibited good adsorption towards Ru, Rh, and Pd with the uptake rates over 95% at 55 °C in 0.1 M HNO 3 –3 M NaNO 3 solution and no adsorption towards 238 U(VI). The adsorption towards Ru, Rh, and Pd matched well with pseudo-second-order model with the equilibrium obtained within 24 h, 24 h and 0.5 h and Langmuir adsorption isotherm model with the saturation adsorption amounts as high as 0.37 mmol/g, 0.34 mmol/g and 0.71 mmol/g respectively. The adsorbed Pd, Rh, and Ru can be desorbed by 0.1 M HNO 3 –0.1 M thiourea , 2 M HCl and NaClO solution (CP) which is expected to realize their mutual separation in desorption stage using the above-mentioned eluents successively. Both FT-IR and XPS revealed that C N C played key role during adsorption and the adsorption needed the participation of NO 3 − to keep charge balance. In a word, iso Bu-BTP/SiO 2 -P is a promising adsorbent for separation and recovery Ru, Rh, and Pd, especially in the case of separating them from other fission products and actinides from high level liquid waste .
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）