CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Fangjun Shao,Zihao Yao,Yijing Gao,Qiang Zhou,Zhikang Bao,Guilin Zhuang,Xing Zhong,Chuan Wu,Zhongzhe Wei,Jianguo Wang
The development of bifunctional catalysts for the efficient hydrogenation and acceptorless dehydrogenation of N -heterocycles is a challenge. In this study, Ru 2 P/AC effectively promoted reversible transformations between unsaturated and saturated N -heterocycles affording yields of 98% and 99%, respectively. Moreover, a remarkable enhancement in the reusability of Ru 2 P/AC was observed compared with other Ru-based catalysts. According to density functional theory calculations, the superior performance of Ru 2 P/AC was ascribed to specific synergistic factors, namely geometric and electronic effects induced by P. P greatly reduced the large Ru-Ru ensembles and finely modified the electronic structures, leading to a low reaction barrier and high desorption ability of the catalyst, further boosting the hydrogenation and acceptorless dehydrogenation processes.
研究领域:
催化化学
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材料科学
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理论化学
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2018
·
IF 0
Tingting Liu,Bomin Feng,Xiuju Wu,Yanli Niu,Weihua Hu,Chang Ming Li
It is desirable yet challenging to develop highly active and durable hydrogen evolution reaction (HER) electrocatalysts with Pt-comparable activity for future energy devices. In this work, we report Ru2P nanoparticle decorated P/N dual-doped carbon nanofibers on carbon cloth (Ru2P@PNC/CC-900) as a highly efficient and durable hierarchical HER electrocatalyst in both acidic and alkaline media. Electrochemical tests show that this Ru2P@PNC/CC-900 possesses Pt-comparable HER activity to support 10 mA cm–2 HER current density at low overpotential of 15 and 50 mV in acidic and alkaline condition, respectively. Density functional theory calculations reveal that coupling Ru2P nanoparticles with heteroatom-doped carbon fibers leads to enhanced intrinsic HER activity. The integrative hierarchical architecture further endows high surface areas with good mechanical robustness to support abundant catalytically active sites and possesses excellent electrical conductivity and efficient access for mass transportation to facilitate the HER process.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
Science China-Materials
·
2022
·Vol. 65
·期 10
·2675-2684
·
IF 8.64
Wei Yue,Xu Gao,Wei Yujie,Ji Lvlv,Wang Tao,Liu Zhun,Wang Sheng
Developing highly efficient, cost-effective, and stable electrocatalysts for hydrogen evolution reaction (HER) is of considerable importance but remains challenging. Herein, we report the fabrication of a robust Ru-based electrocatalyst, which comprises heterostructured Ru-Ru 2 P nanoparticles that are embedded in the N,P-codoped carbon nanofibers (CNFs), through a synthetic strategy involving electrospinning and temperature-controlled pyrolysis treatment. The as-prepared Ru-Ru 2 P catalyst (Ru-Ru 2 P@CNFs) shows excellent HER catalytic activities with low overpotentials of 11 and 14 mV in acidic and alkaline media, respectively, to achieve a current density of 10 mA cm −2 , which are superior to the individual components of pure Ru and Ru 2 P catalysts. Density functional theory calculations demonstrate the existence of electronic coupling effect between Ru and Ru 2 P at the heterointerfaces, leading to a well-modulated electronic structure with optimized hydrogen adsorption strength and enhanced electrical conductivity for efficient HER electrocatalysis. In addition, the overall synthetic strategy can be generalized for the synthesis of a series of transitional metal phosphide-based nanofibers, thereby holding a remarkable capacity for various potential applications.
研究领域:
材料科学
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化学工程
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电化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Jie Liu,Jinhong Ren,Yunmei Du,Xiao Chen,Mengmeng Wang,Yanru Liu,Lei Wang
It is a great challenge to induce the formation of the RuP 4 phase and realize the construction of a metal-rich phase/phosphorus-rich phase-ruthenium phosphide heterostructure by directional regulation of the proportion of P and metal atoms. The ultra-high conductivity of Ru 2 P and the excellent ability of V-doped RuP 4 to absorb/desorb H* are confirmed by density functional theory (DFT) calculations, which laid a theoretical foundation for the construction of a unique Ru 2 P/V-RuP 4 structure to accelerate HER reaction kinetics. This work innovatively uses the V-doping strategy to induce the formation of RuP 4 phase with high intrinsic activity, and finally construct V-Ru x P y nanosheets with rich Ru/Ru 2 P/V-RuP 4 heterostructures. Thanks to the rich Ru/Ru 2 P/V-RuP 4 heterostructure and the optimization of V dopants, the V-Ru x P y catalyst only needs 180 mV to obtain an industrial-grade current density of 1 A cm −2 . In summary, this work provides a new idea for the design and performance optimization of ruthenium-based catalysts.
研究领域:
材料科学
·
催化
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 33
·7826-7830
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IF 5.16
Tingting Liu,Jianmei Wang,Changyin Zhong,Shiyu Lu,Wenrong Yang,Jian Liu,Weihua Hu,Chang Ming Li
Graphical A fair comparison : A strategy to grow nanoparticles of three Ru phosphides on graphene sheets was developed. The resulting three electrocatalysts for the hydrogen evolution reaction (HER; see figure) show similar morphology, loading density, nanoparticle size, Ru content, and electrochemical surface area, which allows a fair comparison of the effect of the phosphide phase on HER activity. Ru 2 P/graphene shows the best HER performance and highest intrinsic activity in acid solution, and all three electrocatalysts show excellent long-term HER durability. The outstanding electrocatalytic activity of ruthenium (Ru) phosphides toward the hydrogen evolution reaction (HER) has received wide attention. However, the effect of the Ru phosphide phase on the HER performance remains unclear. Herein, a two-step method was developed to synthesize nanoparticles of three types of Ru phosphides, namely, Ru 2 P, RuP, and RuP 2 , with similar morphology, dimensions, loading density, and electrochemical surface area on graphene nanosheets by simply controlling the dosage of phytic acid as P source. Electrochemical tests revealed that Ru 2 P/graphene shows the highest intrinsic HER activity, followed by RuP/graphene and RuP 2 /graphene. Ru 2 P/graphene affords a current density of 10 mA cm −2 at an overpotential of 18 mV in acid media. Theoretical calculations further showed that P-deficient Ru 2 P has a lower free energy of hydrogen adsorption on the surface than other two, P-rich Ru phosphides (RuP, RuP 2 ), which confirms the excellent intrinsic HER activity of Ru 2 P and is consistent with experiment results. The work reveals for the first time a clear trend of HER activity among three Ru phosphide phases.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2022
·
IF 12.92
Dan Zhang,Hongfu Miao,Xueke Wu,Zuochao Wang,Huan Zhao,Yue Shi,Xilei Chen,Zhenyu Xiao,Jianping Lai,Lei Wang
In this study, an ultra-fast and simple solvent-free microwave method was successfully demonstrated using a series of ultra-small (~2.5 nm) surfactant-free Ru 2 P@Ru/CNT heterostructures for the first time. The structure has a high-density Ru component and Ru 2 P component interface, which accelerates the hydrogen evolution reaction (HER). The prepared Ru 2 P@Ru/CNT demonstrated excellent catalytic effects for the HER in alkaline media and real seawater. The experimental results indicate that ratio-optimized Ru 2 P@Ru/CNT (Ru 2 P:Ru = 66:34) requires only 23 and 29 mV to reach 10 mA cm –2 in 1.0 mol/L KOH and real seawater, respectively. These values are 10 and 24 mV lower than those of commercial Pt/C in 1.0 mol/L KOH (33 mV) and real seawater (53 mV), respectively, making it among the best non-Pt HER reported in the literature. Additionally, the TOF of Ru 2 P@Ru/CNT in alkaline freshwater and seawater were 13.1 and 8.5 s –1 , respectively. These exceed the corresponding values for Pt/C, indicating that the catalyst has excellent intrinsic activity. The high current activity of Ru 2 P@Ru/CNT in 1.0 mol/L KOH was explored, and only 77 and 104 mV were required to reach 500 and 1000 mA cm –2 , respectively. After 100 h of durability testing, the catalyst retained excellent catalytic and structural stability in low current density, high current density, and seawater.
研究领域:
材料科学
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化学工程
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Longyang Liu,Zichen Wang,Xueyan Zhang,Lijie Luo,Yongjun Chen
Highly active and stable electrocatalysts are highly desired for the hydrogen evolution reaction (HER) in water electrolysis. In this study, a ruthenium-ruthenium phosphide heterojunction (Ru-Ru 2 P) anchored on phosphorus-doped graphene (PCSG) was fabricated via a mild molten salt template method. The graphene was synthesized from discarded coconut shells sourced from Hainan. We found that the heterojunction structure could accelerate electron transfer, while the graphene provided more exposed active sites, significantly enhancing the HER activity of the catalyst. The catalyst prepared at 800 °C with 30 mg of RuCl 3 (Ru-Ru 2 P/2D-PCSG-800) exhibited low HER overpotentials of 31 mV in alkaline and 57 mV in acidic electrolytes at a current density of 10 mA cm −2 , respectively, which were comparable to those of commercial 20 % Pt/C catalyst (36 mV in alkaline and 40 mV in acidic electrolytes). Moreover, the catalyst demonstrated high stability with no significant change in current density after 125 hours of operation. Density functional theory calculations revealed that the Ru-Ru 2 P heterojunction could rearrange charge and modify the Ru d -band center, optimizing the adsorption energy of active *H (|ΔG *H |) and breakage energy of *H-OH bond (ΔG H2O ).
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2026
·
IF 9.2
Dan Zhang,Jin Liu,Bin Song,Chenyu Li,Yuyao Chen,Huaifang Zhang,Yuanyuan Feng
“Time-amount” precise phosphidation successfully constructs amorphous/crystalline/metallic three-phase heterojunction. • Multiphase heterojunction functional synergy facilitates the spatial division of labor for HER pathway at the nanoscale. • Ru→Ru 2 P→a-Ru 2 P relay electron transfer mechanism ensures its excellent seawater HER at industrial current density. Sluggish water dissociation kinetics and stability issues caused by chloride ions pose severe challenges for hydrogen evolution reaction (HER) catalysts in alkaline seawater environments. This study proposes a design philosophy of “multiphase heterojunction functional synergy”. Through a precise microwave phosphidation strategy, a three-phase heterojunction catalyst composed of amorphous Ru 2 P, crystalline Ru 2 P, and metallic Ru (a/c-Ru 2 P@Ru/C) was successfully synthesized. Systematic modulation enabled controllable synthesis of the catalyst's microstructure (amorphous/crystalline phase ratio) and macroscopic composition. This catalyst demonstrates outstanding comprehensive performance in alkaline seawater media: it exhibits a low overpotential of only 36 mV at a current density of 10 mA cm −2 , maintains stable operation for over 200 h at a high current density of 500 mA cm −2 , and shows leading cell voltage for overall water splitting. A series of characterizations indicate that the successful formation of a three-phase heterostructure in a/c-Ru 2 P@Ru/C induces interfacial electron transfer from Ru to phosphides, thereby optimizing the electronic structure of active sites. This multiphase synergy achieves a “spatial division of labor” in the HER reaction pathway: electron-rich amorphous regions promote water dissociation, while electron-modulated metallic sites accelerate hydrogen desorption. Concurrently, the robust heterointerface ensures long-term stability under harsh seawater conditions.
✓ 已验证
DOI
高影响因子
Materials Horizons
·
2023
·Vol. 10
·期 12
·5712-5719
·
IF 13.3
Mengmeng Wang,Yunmei Du,Shuangshuang Li,Xiaoli Sun,Bin Li,Yuanxiang Gu,Lei Wang
The N-doping strategy plays a vital role in optimizing electrocatalytic performance, but it often requires high-temperatures accompanied by the emission of irritating gases, which is contrary to the concept of energy saving and environmental protection. Based on this, this work innovatively uses the quenching of waste heat and the non-equilibrium state of materials to realize controllable N-doping. Notably, N dopants stimulate metal-like electroconductivity and accelerate the alkaline HER kinetics by optimizing the electronic structure of Ru2P. Surprisingly, the hydrophilic Ru core and the N-Ru2P shell with a low HER reaction energy barrier synergistically expedite hydrogen release. As anticipated, the current density of N-Ru2P@Ru (963 mA cm−2) is 2.6-fold that of Pt/C (359 mA cm−2) at 150 mV. Overall, the novel N-doping technology greatly simplifies material preparation procedures and reduces energy consumption. Moreover, this unique N-doping strategy provides a new idea for optimizing the catalyst structure and reaction kinetics.
研究领域:
材料科学
·
电催化
·
能源技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）