INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
·
IF 2.495
Xiaodong Huang,YanEn Wang,Qinshu Zhu,Kejie Zhou,Huizhen Zhi,Jinfei Yang
Hydrazine hydrate oxidation assisted water splitting can effectively reduce the energy consumption of conventional water electrolysis due to the lower thermodynamic anode potential, which stimulates the development of highly efficient bifunctional electrocatalysts. Herein, we report a solvothermal synthesis strategy to prepare Rh nanocubes (NCs) with specific exposed Rh (1 0 0) planes. Benefiting from higher coordination unsaturation and reactivity of the Rh (1 0 0) plane, Rh NCs exhibit higher catalytic performance than commercial Rh black toward hydrazine hydrate oxidation reaction (HHOR) and hydrogen evolution reaction (HER). To achieve the current density of 10 mA cm −2 in HHOR and HER, the anode and cathode potentials required for Rh NCs (240 and –32 mV) are better than those of commercial Rh black (291 and −43 mV). Thus, Rh NCs are used as bifunctional electrocatalysts to drive a HHOR assisted water splitting cell, which can achieve long-term stable electrochemical hydrogen production at a voltage of ∼ 0.223 V, demonstrating a promising energy-saving hydrogen production strategy.
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2021
·Vol. 15
·期 2
·1288-1294
·
IF 8.897
Guo Xiaoyun,Hu Zheng,Lv Jianxin,Li Hui,Zhang Qinghua,Gu Lin,Zhou Wei,Zhang Jiangwei,Hu Shi
Metal catalysts play an important role in the catalytic electrochemical processes and optimization of their performance is usually achieved through alloying with other metal atoms. Doping with interstitial hydrogen atoms is a special but effective way to regulate the electronic structure of host catalysts. Herein we demonstrate the intermixing of Pd and Rh atoms during the hydrogen-doping process of Pd@Rh core-shell nanocubes, forming an alloyed surface in Pd@Rh-H. The catalysts show enhanced performance in electrocatalytic methanol oxidation, as compared to commercial Pt/C and are even better than PdH@Rh core-shell nanocubes. The small structural differences between the two hydride catalysts are revealed by X-ray electron spectroscopy and pair distribution function analysis of electron diffraction. The theoretical calculation results show that Rh in Pd@Rh-H contains more negative charges than Rh in PdH@Rh, indicating more effective charge transfer in Pd@Rh-H. The d-band center ( ε d ) of the Rh site in Pd@Rh-H shifts up, and the synergy between Rh and Pd optimizes the binding energy of CO and OH, inducing preferential catalytic activity. Our work provides guidance for the synthesis of high-performance catalysts by doping with interstitial atoms, which may provide a new strategy to fine-tune the electronic structure of other bimetallic nanoparticles.
✓ 已验证
产品关联
DOI
高影响因子
Chemistry-An Asian Journal
·
2020
·Vol. 15
·期 20
·3356-3364
·
IF 4.056
Kai Liu,Zixi Lyu,Xuejiao Chen,Xinyan Liao,Guanhong Chen,Xin Lin,Wei Wang,Shuifen Xie
Graphical A selective synthesis of atypical Rh−Pt alloyed nanocrystals with different morphologies and defective structures has been achieved through kinetically manipulating the nucleation and nucleus attachment. The defective Rh 47 Pt 53 wavy nanowires endowed with abundant grain boundaries and twin boundaries present a superior electrocatalytic performance for the ethanol oxidation reaction. Defective metal nanostructures have attracted great attention due to the striking catalytic behavior of the defect sites. Atypical metal nanocrystals generated from attached nuclei can accommodate abundant grain boundaries (GBs) and twin boundaries (TBs). However, the understanding of their growth-mechanism and precisely synthetic control over such defective nanocrystals are still scarce. Herein, using the Rh−Pt nanoalloy as a model system, we systematically demonstrate that a prudent control of the reaction kinetics can manipulate the metal nucleation and nucleus attachment to create atypical nanocrystals, including small isolated nanoparticles (NPs), defect-rich wavy nanowires (WNWs), and {100} facet-bounded spliced nanocubes (SNCs). In the ethanol oxidation electrocatalysis, the Rh 47 Pt 53 WNWs featured with abundant TBs and GBs show the greatest mass activity (0.655 A ⋅ mg −1 Pt , 2.9 times to the commercial Pt/C) and durability. Our work captures the core of reaction kinetics on regulating the nucleus attachment and enables the rational control over the nanocrystal morphology and defect.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2020
·
IF 6.146
Zhou Ren,Yang Liu,Yuan Lyu,Xiangen Song,Changyong Zheng,Zheng Jiang,Yunjie Ding
A single-Rh-site catalyst (Rh-TPISP) that was ionically-embedded on a P(V) quaternary phosphonium porous polymer was evaluated for heterogeneous ethanol carbonylation . The [Rh(CO)I 3 ] 2– unit was proposed to be the active center of Rh-TPISP for the carbonylation reaction based on detailed Rh L 3 -edge X-ray absorption near edge structure (XANES), X-ray photoelectron spectroscopy (XPS), and Rh extended X-ray absorption fine structure (EXAFS) analyses. As the highlight of this study, Rh-TPISP displayed distinctly higher activity for heterogeneous ethanol carbonylation than the reported catalytic systems in which [Rh(CO) 2 I 2 ] − is the traditional active center. A TOF of 350 h −1 was obtained for the reaction over [Rh(CO)I 3 ] 2– , with >95% propionyl selectivity at 3.5 MPa and 468 K. No deactivation was detected during a near 1000 h running test. The more electron-rich Rh center was thought to be crucial for explaining the superior activity and selectivity of Rh-TPISP, and the formation of two ionic bonds between [Rh(CO)I 3 ] 2– and the cationic P(V) framework ([P] + ) of the polymer was suggested to play a key role in firmly immobilizing the active species to prevent Rh leaching.
✓ 已验证
产品关联
DOI
高影响因子
Biomaterials Science
·
2020
·Vol. 8
·期 15
·4157-4165
·
IF 6.183
Mengli Ding,Zhaohua Miao,Fan Zhang,Jie Liu,Xintao Shuai,Zhengbao Zha,Zhong Cao
Catalytic nanomedicine with high oxygen-generation efficiency may find applications in alleviating tumor hypoxia and improving the efficiency of photodynamic therapy (PDT). In this study, a catalytic nanosystem (Ce6-Rh@MPDA) was developed using mesoporous polydopamine nanoparticles (MPDA) to encapsulate catalase-like rhodium nanoparticles (Rh NPs) and photosensitizer chlorine6 (Ce6) for photoacoustic/fluorescence dual imaging-guided tumor therapy. The Rh NPs can catalyze the production of O2 from tumor-enriched H2O2in situ, in which the mesoporous structure of MPDA plays an important role via improving the catalytic efficiency of Rh NPs. Moreover, the hyperthermia generated by both MPDA and Rh NPs under laser irradiation accelerates the O2 generation to promote the PDT. The Ce6-Rh@MPDA nanoparticles described herein represent a multifunctional metal-based catalytic nanomedicine which not only alleviates tumor hypoxia but also enables a synergistic antitumor treatment using PTT and PDT.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Man Yang,Yuxiang Jiao,Jianglin Duan,Keying Wu,Hailiang Song,Shaodong Sun,Yujing Ren
Taking the background of the ambiguous role of oxophilic metal oxide in metal-acid bifunctional catalysts for the important field of tetrahydrofurfuryl alcohol (THFA) hydrogenolysis, a linear relationship between the W═O/W–OH content in sub-nano-Rh-supported WOx and 1,5-pentanediol (1,5-PeD) yields from THFA hydrogenolysis has been established. It reveals that the higher reduction temperature promotes the surface Rh/W ratio. Thus, hydrogen spillover is facilitated, leading to more surface W═O structures and thereby more in-situ-reduced W–OH generation. W–OH structures work as the active sites to provide in situ Brønsted acid, resulting in enhanced selective activation for secondary C–O bonds of THFA. This discovery reveals the unique role of the surface structure on oxophilic metal oxide in chemoselective hydrogenolysis of the secondary C–O bond in polyols.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Research
·
2021
·
IF 0
Yuqing Cheng,Jiafu Shi,Yizhou Wu,Xueying Wang,Yiying Sun,Ziyi Cai,Yu Chen,Zhongyi Jiang
Solar-driven photocatalytic regeneration of cofactors, including reduced nicotinamide adenine dinucleotide (NADH), reduced nicotinamide adenine dinucleotide phosphate (NADPH), and reduced flavin adenine dinucleotide (FADH2), could ensure the sustainable energy supply of enzymatic reactions catalyzed by oxidoreductases for the efficient synthesis of chemicals. However, the elevation of cofactor regeneration efficiency is severely hindered by the inefficient utilization of electrons transferred on the surface of photocatalysts. Inspired by the phenomenon of ferredoxin-NADP+ reductase (FNR) anchoring on thylakoid membrane, herein, a homogeneous catalyst of rhodium (Rh) complex, [Cp∗Rh(bpy)H2O]2+, was anchored on polymeric carbon nitride (PCN) mediated by a tannic acid/polyethyleneimine (TA/PEI) adhesive layer, acquiring PCN@TA/PEI-Rh core@shell photocatalyst. Illuminated by visible light, electrons were excited from the PCN core, then transferred through the TA/PEI shell, and finally captured by the surface-anchored Rh for instant utilization during the regeneration of NADH. The TA/PEI-Rh shell could facilitate the electron transfer from the PCN core and, more importantly, achieved ~1.3-fold elevation of electron utilization efficiency compared with PCN. Accordingly, the PCN@TA/PEI-Rh afforded the NADH regeneration efficiency of 37.8% after 20 min reaction under LED light (405 nm) illumination, over 1.5 times higher than PCN with free Rh. Coupling of the NADH regeneration system with formate dehydrogenase achieved continuous production of formate from carbon dioxide (CO2). Our study may provide a generic and effective strategy to elevate the catalytic efficiency of a photocatalyst through intensifying the electron utilization.
研究领域:
生物化学
·
光催化材料科学
✓ 已验证
DOI
Inorganic Chemistry Frontiers
·
2025
·
IF 6.4
Guangxia Wang,Wenhui Wang,Yaozhong Yu,Tao Hu,Juan Ding,Yongming Sui
Active and durable catalysts are crucial for the hydrogen evolution reaction (HER). In the volcano plot, rhodium (Rh) and platinum (Pt) are positioned closely, while the activity and stability of Rh are much inferior to those of Pt. Here, we developed a Rh/TiO2/Ti electrocatalyst to mitigate Pt dependency. The in situ formed TiO2 with oxygen vacancies was prepared utilizing Ti foam as the Ti source. The TiO2 support can confine Rh nanoparticles and ensure charge accumulation at the Rh site, while Rh can enhance the conductivity of TiO2. DFT calculations demonstrate that the strong interaction between Rh and TiO2 could regulate the electronic structure of Rh, thereby accelerating water dissociation and optimizing the adsorption strength of *H. Consequently, compared to Rh/Ti, Rh/TiO2/Ti exhibits significantly enhanced HER activity, requiring overpotentials of only 37.3 and 34.3 mV to reach 10 mA cm−2 in the alkaline and acidic HER, respectively. Furthermore, the vertical nanoarray structure, surface roughness, and metal–support interaction endow Rh/TiO2/Ti with remarkable durability. It works in both alkaline and acidic media for 120 hours at 10 mA cm−2 with unnoticeable activity decline, outperforming commercial Pt/C. This work provides a strategy to overcome the activity and stability limitations of Rh-based catalysts, providing references for promising catalysts for water electrolysis.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2026
·
IF 7.8
Taiping Fu,Zekun Jing,Xinrong Yan,Yongsheng Li,Biye Niu,Zhanpeng Ye,Yufeng Liu,Yakun Guo,Maobing Shuai
Achieving the highly efficient hydrogenation of polycyclic aromatic hydrocarbons (PAHs) under mild temperatures remains a significant challenge. Herein, we report a highly active RuRh alloy catalyst supported on carbon nanofibers (RuRh/CNFs) developed via element screening. This catalyst achieves 100% conversion of naphthalene to decalin within 15 min at room temperature under solvent-free conditions. It exhibits a high turnover frequency (TOF) of 214.2 h–1 at 25 °C (1071 h–1 at 35 °C), significantly surpassing single-metal catalysts. Additionally, a 97% yield of the intermediate tetralin was obtained by fine-tuning the kinetic parameters. The catalyst demonstrates exceptional recyclability and broad substrate universality. Mechanistic studies attribute this performance to the synergistic effect between Ru and Rh, which enhances hydrogen migration and optimizes adsorption energies for substrates and intermediates, providing both theoretical insights and practical validation for the rational design of highly efficient PAHs as hydrogenation catalysts.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2025
·
IF 8.4
Chengqi Feng,Anran Li,Yuxin Zhu,Yan Lei,Chenkai Jin,Juncheng Huang,Haining Na,Jin Zhu
Polluted water poses a significant threat to human health and ecological balance, necessitating the development of efficient and cost-effective water purification technologies. This study synthesized a composite photocatalytic material (CMF@Fe x O y -CN) using a microwave radiation synchrotron cooling technique. This material incorporates iron oxide-doped g-C 3 N 4 and in-situ micro-fibrillated cellulose, exhibiting high dispersion stability and magnetic recyclability. The material demonstrates a bandgap energy ( E g ) of 2.69 eV. Remarkably, 25 mg/20 mL of CMF@Fe x O y -CN (with 40 wt% Fe x O y -CN loading) achieved a 97.9 % degradation of Rhodamine B (Rh B) within 1 h. Even after 10 cycles, the degradation efficiency remained high at 89.4 %. The superoxide radical (·O 2 − ) played a critical role in Rh B degradation, facilitated by the stable dispersion of CMF. The issue of low photocatalytic efficiency, often caused by poor dispersion of photocatalysts, was addressed through the in-situ micro-fibrillation of cellulose, offering a green and economical solution. This study provides a theoretical foundation for applying photocatalysis in water purification.
研究领域:
环境科学
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
IF 5.951
Yueling Cao,Minghui Tang,Mingming Li,Jiang Deng,Fan Xu,Lei Xie,Yong Wang
A novel N-doped carbon supported Rh catalyst was developed via one-pot pyrolysis of chitin and (NH4)3RhCl6. The catalyst exhibited excellent catalytic activity and recyclability for the hydrogenation of benzoic acid to cyclohexane carboxylic acid. Characterization indicated that the high catalytic performance of Rh/N–C-700 is mainly attributed to the proportion of Rh0 to Rh3+ and Rh particle size. More importantly, this novel synthesis strategy significantly increased the interaction between Rh nanoparticles and N-doped carbon in contrast with the conventional impregnation and NaBH4 reduction methods, thus preventing the Rh nanoparticles from migration, aggregation, and leaching from the support surface and therefore improving the reusability of the catalyst. This synthetic method may pave a new way for producing N-doped carbon supported metal catalysts from chitin on a large scale, which is attractive for industrial applications.
研究领域:
化学工程
·
材料科学
·
催化反应
✓ 已验证
DOI
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Mingjing Ma,Huanhuan Yu,Baolin Zhu,Wenjun Zheng,Shoumin Zhang
The design of efficient catalysts with atom clusters (ACs) and single atoms (SAs) as active sites for water splitting presents an effective approach for improving bifunctional electrocatalytic performance by synergistically promoting electron transport and proton transfer kinetics. In this work, a series of Fe2O3-supported noble metal catalysts (M = Ru, Rh, Pd, Ag) incorporating both ACs and SAs sites were developed, with detailed characterization identifying Ru ACs as the primary active centers. The designed-interfacial M-O-Fe bonds play a critical role in charge redistribution, subsequently enhancing electron and proton transfer kinetics. The resulting heterostructure optimizes both the electronic environment and active site accessibility, yielding exceptional electrocatalytic performance. Further density functional theory calculations demonstrate that the incorporation of Ru species leads to increased filling of antibonding orbitals and modulation of the d-band center, subsequently reducing the energy barrier of the rate-determining steps to −0.267 eV for HER and 1.522 eV for OER, respectively. Consequently, the representative Ru/Fe2O3 with Ru content of 1.1 wt.% achieves an OER overpotential of 189 mV and a HER overpotential of 21 mV at a current density of 10 mA cm−2. This study highlights a novel approach to the design of advanced bifunctional electrocatalysts by engineering interfacial bridge bonds.
研究领域:
电化学
·
催化
·
材料科学
·
纳米技术
·
理论化学
✓ 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）