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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Quenching induces the co-introduction of O vacancies and N dopants in Co-RuO2 to promote ampere-level current density hydrogen production

Yilin Wang,Xiaoli Sun,Yunmei Du,Shuangshuang Li,Mengmeng Wang,Yanru Liu,Lei Wang

Optimizing the electronic structure of Ru by introducing N dopants or O vacancies (V O ) into RuO 2 is expected to be a promising strategy to stimulate the hydrogen evolution reaction (HER) performance. However, it is a challenge to develop a fast and low-energy method to simultaneously achieve the construction of N dopants and V O . This work was the first to optimize the quenching technique for achieving the co-introduction of V O and N in Co-RuO 2 nanosheets (N,Co-RuO 2 -V O ). Related characterizations confirmed that V O and N dopants synergistically optimized the electronic configuration of Ru and the reaction path of alkaline HER. As expected, the mass activity of N,Co-RuO 2 -V O (2208.63 mA m g R u - 1 ) was 8.05-fold that of Pt/C at 100 mV for alkaline HER. Surprisingly, N,Co-RuO 2 -V O required only 148.6 mV to achieve an industrial-grade current density of 1 A cm −2 , which was much lower than the commercial Pt/C catalyst (312 mV). Overall, this work provides an energy-efficient new strategy for the development of Ru-based catalysts with ampere-level currents.

CAS / MDL: 14898-67-0
研究领域: 材料科学 · 电化学 · 催化
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DALTON TRANSACTIONS · 2020 ·Vol. 49 ·期 37 ·13152-13159 · IF 4.174

Regulating the electronic structure of CoMoO4 microrod by phosphorus doping: an efficient electrocatalyst for the hydrogen evolution reaction

Feixiang Jiao,Jinhui Li,Jinlei Wang,Yu Lin,Yaqiong Gong,Xiaofei Jing

It is of extreme importance to design efficient electrocatalysts for hydrogen evolution reaction (HER), which is considered as a promising approach to provide efficient and renewable clean fuel (hydrogen). Tuning the electronic structure through heteroatom doping demonstrates one of the most effective strategies to promote the electrocatalytic performance of HER. Herein, phosphorus-doping modulation is utilized to fabricate monoclinic P-CoMoO4 with optimized electron structure supported on nickel foam (P-CoMoO4/NF) for alkaline HER via a facile hydrothermal method, followed by low-temperature phosphidation. Notably, P-CoMoO4/NF shows outstanding electrocatalytic performance for HER in 1 M KOH with a low overpotential of 89 mV at 10 mA cm−2, a remarkable Tafel slope value of 59 mV dec−1, and excellent 24 h-long stability. The excellent catalyst activity and stability merits of P-CoMoO4/NF are comparable to the reported highly efficient non-precious metal HER electrocatalysts and could be applied as a powerful electrocatalyst in water electrolysis. This work provides a superior synthesis strategy for the effective design and rational fabrication of low-cost, highly active, and highly stable non-precious metal HER electrocatalysts for electricity-to-hydrogen applications.

CAS / MDL: 31175-20-9 7440-06-4
研究领域: 材料科学 · 电化学 · 可再生能源
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ACS Nano · 2019 · IF 13.903

Interstitial Hydrogen Atom Modulation to Boost Hydrogen Evolution in Pd-Based Alloy Nanoparticles

Jinchang Fan,Xiaoqiang Cui,Shansheng Yu,Lin Gu,Qinghua Zhang,Fanqi Meng,Zhangquan Peng,Lipo Ma,Jing-Yuan Ma,Kun Qi,Qiaoliang Bao,Weitao Zheng

Rational control of the components of noble metal alloys is paramount for achieving satisfactory electrocatalytic performances. Though transition metals are commonly used to modify noble metals, many potential elements remain to be explored. Here, we interstitially modulate hydrogen atoms into RhPd nanoparticles to boost the alkaline hydrogen evolution reaction (HER). The obtained stable RhPd-H nanoparticles exhibit pronounced alkaline HER activity with a small overpotential of 36.6 mV at 10 mA cm–2 and a low Tafel slope of 35.3 mV dec–1. The surface electronic state, bond distance, and coordination number of the Rh and Pd atoms are significantly influenced by the presence of interstitial hydrogen atoms. These modifications give RhPd-H nanoparticles a desirable hydrogen adsorption free energy, thus accelerating the hydrogen gas production. We further demonstrate that the interstitial hydrogen atom modulation strategy to improve the HER activity is universal for other Pd-based alloy nanostructures. This work presents a powerful strategy for designing efficient electrocatalysts for the HER and beyond.

CAS / MDL: 14284-92-5
研究领域: 材料科学 · 电化学 · 催化
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APPLIED CATALYSIS B-ENVIRONMENTAL · 2024 · IF 20.2

Strain regulation of bond length in single Ru sites via curving support surface for enhanced hydrogen evolution reaction

Yan Liu,Liwen Xing,Yaqi Liu,Dianxing Lian,Mohaoyang Chen,Weiwei Zhang,Ke Wu,Hongdan Zhu,Zhiyi Sun,Wenxing Chen,Peng Wu,Dingsheng Wang,Yongjun Ji

The intrinsic activity of single-atom catalysts is influenced by the local electronic structures of metal centers, with existing modulation strategies limited to adjacent atomic coordination. However, the impacts of support surface geometry on local bonding environment, and thus electronic structures of single-atom centers have rarely been known. Here, we prepared highly curved B,N co-doped carbon-supported ruthenium catalyst with an ultra-low Ru loading of 0.4 wt%, which exhibited an ultrahigh turnover frequency (TOF) of 10 H 2 s −1 (38 times that of Pt/C) and superior stability in alkaline hydrogen evolution reaction (HER). We found that curving support surface induced the strain, resulting in 1.5% compressed Ru-N and 4% stretched Ru-B bonds, leading to the accumulation of positive charge and quenching of spin polarization at Ru sites, thereby achieving the optimal binding of H* and enhanced performance for HER. This work highlights the significant support effects upon the structural design of active sites.

CAS / MDL: 13746-66-2 14459-95-1
研究领域: 催化 · 材料科学 · 化学 · 能源科学
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ACS Applied Nano Materials · 2022 · IF 6.14

NiMo-Based Nanorod Arrays Supported on Ni Foams for Efficient Hydrogen Electrocatalysis

Yunfang Yan,Xuejie Cao,Liangmin Ning,Fei Lin,Wenzhuo Qin,Xin Liu,Wen Gu

The construction of low-cost electrocatalysts with good conductivity, excellent intrinsic activity, and superior stability is crucial for the hydrogen evolution reaction (HER). Herein, we report an outstanding catalyst (Ni0.2Mo0.8N/NiMoP2/MoO2@NC) consisting of NiMo-based nanorod arrays supported on Ni foams for the efficient alkaline HER. It shows an ultralow overpotential of 48 mV and remarkable longevity for over 145 h at 10 mA cm–2 in 1.0 M KOH. The integration of ample compositions is favorable to the formation of heterointerfaces, accelerating electron transfer. The assembly of transition metal nitrides and phosphides fully develops the electrical conductivity of metal materials, which paves the way for superstability. The superior electrocatalytic activities can be attributed to the vital features, including the synergistic effect of Ni0.2Mo0.8N and NiMoP2, good electrical conductivity of MoO2, and corrosion resistance of NC basement. The present work proposes that regulating compositions and hierarchical nanostructures are of significance in developing electrode materials for the HER.

CAS / MDL: 7440-06-4
研究领域: 材料科学 · 电化学 · 催化 · 能源材料
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