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Single-atom Co alloyed Ru for electrocatalytic nitrite reduction to ammonia

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Nano Research 2024年第5期17卷 3660-3666页

作者： Fuzhou Wang Jiaqi Xiang Guike Zhang Kai Chen ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrochemical converting NO_(2)^(-)into NH_(3)(NO_(2)RR)holds an enormous prospect to attain efficient NH_(3) electrosynthesis and polluted NO_(2)^(-)***,we report single-atom Co alloyed Ru(Co_(1)Ru)as an efficient and durable NO_(2)RR *** experimental and theoretical investigations reveal that single-atom Co alloying of Ru enables the construction of Co_(1)-Ru heteronuclear active sites to synergistically promote NO_(2)^(-)activation/hydrogenation while suppressing the competitive H_(2) evolution,rendering the greatly enhanced activity and selectivity of Co_(1)Ru towards the NO_(2)***,Co_(1)Ru assembled within a flow cell exhibits an impressive NH_(3) yield rate of 2379.2μmol·h^(-1)·cm^(-2) with an NH_(3)-Faradaic efficiency of 92%at a high current density of 415.9 mA·cm^(-2),which is among the highest NO_(2)RR performances reported to date.

关键词： electrochemical converting NO_(2)-into NH3 single-atom alloys theoretical computations industrial-level current density

Optimization on bicriterion policies for M/G/1 system with second optional service

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Journal of Zhejiang University-Science A(Applied Physics & Engineering) 2008年第10期9卷 1437-1445页

作者： Jau-chuan ke Yunn-kuang chu Department of Applied Statistics National Taichung Institute of Technology Taichung 404 Taiwan China

We compare the optimal operating cost of the two bicriterion policies, and , for an M/G/1 queueing system with second optional service, in which the length of the vacation period is randomly controlled either by the number of arrivals during the idle period or by a timer. After all the customers are served in the queue exhaustively, the server immediately takes a vacation and may operate policy or policy. For the two bicriterion policies, the total average cost function per unit time is developed to search the optimal stationary operating policies at a minimum cost. Based upon the optimal cost the explicit forms for joint optimum threshold values of (p,T) and (p,N) are obtained.

关键词： Average operating cost Bicriterion policy Optimization comparisons Optional service Optimal threshold values

Predicted interfacial thermal conductance and thermal conductivity of diamond/Al composites with various interfacial coatings

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Rare Metals 2011年第5期30卷 544-549页

作者： LIANG Xuebing JIA Chengchang chu ke CHEN Hui School of Materials Science and Engineering University of Science and Technology Beijing Beijing 100083 China General Research Institute for Nonferrous Metals （GRINM） Beijing 100083 China

The interfacial thermal conductance （ITC） and thermal conductivity （TC） of diamond/Al composites with various coatings were theoretically studied and discussed. A series of predictions and numerical analyses were performed to investigate the effect of thickness, sound velocity, and other parameters of coating layers on the ITC and TC. It is found that both the ITC and TC decline with increasing coating thickness, especially for the coatings with relatively low thermal conductivity. Nevertheless, if the coating thickness is close to zero, or quite a small value, the ITC and TC are mainly determined by the constants of the coating material. Under this condition, coatings such as Ni, TiC, Mo 2 C, SiC, and Si can significantly improve the ITC and TC of diamond/Al composites. By contrast, coatings like Ag will exert the negative effect. Taking the optimization of interfacial bonding into account, conductive carbides such as TiC or Mo 2 C with low thickness can be the most suitable coatings for diamond/Al composites.

关键词： metallic matrix composites coatings diamonds thermal conductivity interfacial thermal conductance

FeTe_(2) as an earth-abundant metal telluride catalyst for electrocatalytic nitrogen fixation

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Journal of Energy Chemistry 2021年第5期30卷 259-263页

作者： Yali Guo Yonghua Cheng Qingqing Li ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070GansuChina

Design of cost-effective,yet highly active electrocatalysts for nitrogen reduction reaction(NRR)is of vital significance for sustainable electrochemical NH_(3) ***,we have demonstrated,from both computational and experimental perspectives,that FeTe_(2) can be an efficient and durable NRR *** computations unveil that FeTe_(2) possesses abundant surface-terminated and low-coordinate Fe sites that can activate the NRR with a low limiting potential(-0.84 V)and currently impede the competing hydrogen evolution *** a proof-of-concept prototype,we synthesized FeTe_(2) nanoparticles supported on reduced graphene oxide(FeTe_(2)/RGO),which exhibited a high NRR activity with the exceptional combination of NH_(3) yield(39.2 lg h^(-1) mg^(-1))and Faradaic efficiency(18.1%),thus demonstrating the feasibility of using FeTe_(2) and other earth-abundant metal tellurides for electrocatalytic N_(2) fixation.

关键词： Electrocatalytic nitrogen reduction Fe catalysts Tellurides Density functional theory

Boron Nitride Quantum Dots/Ti_(3)C_(2)T_(x)-MXene Heterostructure For Efficient Electrocatalytic Nitrogen Fixation

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Energy & Environmental Materials 2022年第4期5卷 1303-1309页

作者： ke chu Xingchuan Li Ye Tian Qingqing Li Yali Guo School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China Department of Physics College of ScienceHebei North UniversityZhangjiakou 075000China

Electrocatalytic N_(2) fixation through N_(2) reduction reaction(NRR)has been regarded as a promising route for sustainable NH_(3) synthesis,while exploring high-performing NRR catalysts is pivotal yet ***,BN quantum dots/Ti_(3)C_(2)T_(x)-MXene(BNQDs/Ti_(3)C_(2)T_(x))heterostructure is demonstrated as an efficient and durable NRR catalyst,exhibiting a high NH_(3) yield of 52.8±3.3μg h^(-1) mg^(-1) with an FE of 19.1±1.6%at0.4 V(***),which stand at the high level among all reported BN-and MXene-based NRR *** computations reveal that the electronic interactions between BNQDs and Ti_(3)C_(2)T_(x) enrich the electron density of B atoms at the heterointerface and endow them with enhanced electron-donating capability for N_(2) activation and ***,the decorated BNQDs can block the active sites of Ti_(3)C_(2)T_(x) for hydrogen evolution,rendering a high N_(2)-to-NH_(3) selectivity.

关键词： Boron nitride quantum dots Density functional theory Electrocatalytic nitrogen fixation MXene

Iridium single-atom catalyst for highly efficient NO electroreduction to NH_(3)

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Nano Research 2023年第7期16卷 8737-8742页

作者： Kai Chen Guohui Wang Yali Guo Dongwei Ma ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China key Laboratory for Special Functional Materials of Ministry of Education School of Materials Science and EngineeringHenan UniversityKaifeng 475004China

Atomically dispersed Ir confined in amorphous MoO_(3)(Ir1/a-MoO_(3))was designed as a high-efficiency catalyst for electrochemical reduction reaction of NO to NH_(3)(NORR).Atomic precise characterizations reveal that isolated Ir atoms are immobilized in Ovacancies of amorphous MoO_(3) to form Ir_(1)-O_(5) *** computations demonstrate that single-site Ir1-O5 can not only powerfully activate and hydrogenate NO with a near-zero energy barrier,but also exhibit a higher affinity to NO over H adatoms to suppress the competing hydrogen evolution and promote both NORR activity and ***,Ir_(1)/a-MoO_(3) shows the maximum NH_(3)yield rate of 438.8μmol·h^(-1)·cm^(-2) and NH_(3)-Faradaic efficiency of 93.2%,representing one of the most efficient NORR catalysts to date.

关键词： electrochemical reduction of NO to NH_(3) single-atom catalysts amorphous materials theoretical calculations

MXene Quantum Dots/Copper Nanocomposites for Synergistically Enhanced N_(2)Electroreduction

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Energy & Environmental Materials 2023年第1期6卷 192-198页

作者： Yonghua Cheng Xingchuan Li Peng Shen Yali Guo ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrocatalytic N_(2) reduction reaction(NRR)represents an appealing solution for sustainable ammonia production,whereas exploring high-efficiency NRR catalysts is highly desired but extremely ***,we combine Ti_(3) C_(2)T_(x)-MXene quantum dots(MQDs)with porous Cu nanosheets to design a novel heterostructured MQDs/Cu as an effective and durable NRR ***,MQDs/Cu showed a synergistically enhanced NRR activity with an NH_(3) yield of 78.5 lg h^(-1) mg^(-1)(-0.5 V)and a Faradaic efficiency of 21.3%(-0.4 V),far superior to pure MQDs and Cu,and outperforming the majority of the state-of-the-art NRR *** function theory computations demonstrated that the synergy of MQDs and Cu enabled the creation of interfacial Cu-Ti dimer as dual-active-centers to strongly activate the absorbed N 2 and promote the*N_(2)H formation,consequently resulting in the much reduced energy barriers and greatly enhanced NRR performance.

关键词： density functional theory electrocatalytic nitrogen fixation heterostructure MXene quantum dots

Sulfur-deficient Bi_(2)S_(3-x) synergistically coupling Ti_(3)C_(2)T_(x)-MXene for boosting electrocatalytic N_(2) reduction

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Nano Research 2022年第5期15卷 3991-3999页

作者： Yaojing Luo Peng Shen Xingchuan Li Yali Guo ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrocatalytic nitrogen reduction reaction(NRR)is an appealing route for the sustainable NH_(3)synthesis,while developing efficientand durable NRR catalysts remains at the heart of achieving high-efficiency N_(2)-to-NH_(3)***,we rationally combine vacancy and interface engineering to design sulfur-deficient Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene as an effective NRR *** developed Bi2S3 nanoparticles decorated Ti_(3)C_(2)T_(x)-MXene(Bi2S3-xTi_(3)C_(2)T_(x))naturally contained abundant S-vacancies and exhibited a dramatically boosted NRR activity with an NH_(3)yield of 68.3μg·h^(-1)mg^(-1)(-0.6 V)and a Faradaic efficiency of 22.5%(-0.4 V),far superior to pure Bi_(2)S_(3)and Ti_(3)C_(2)T_(x)and surpassing almost all ever reported Bi-and MXene-based NRR *** investigations unveiled that the exceptional NRR activity of Bi_(2)S_(3-x)/Ti_(3)C_(2)T_(x)stemmed from its dual-active-center system involving both S-vacancies and interfacial-Bi sites,which could synergistically promote N_(2)adsorption and*N_(2)H formation to result in an energetic-favorable NRR process.

关键词： electrocatalytic nitrogen reduction bismuth catalyst MXene vacancy engineering interface engineering

Electrochemical NO reduction to NH3 on Cu single atom catalyst

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Nano Research 2023年第4期16卷 5857-5863页

作者： Kai Chen Guike Zhang Xiaotian Li Xiaolin Zhao ke chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China National Engineering Laboratory for Electric Vehicles Beijing Institute of TechnologyBeijing 100081China

Electrochemical NO reduction reaction(NORR)to generate NH_(3)emerges as a fascinating approach to achieve both NO pollution mitigation and sustainable NH_(3)***,we demonstrate that single-atomic Cu anchored on MoS_(2)(Cu_(1)/MoS_(2))comprising Cu_(1)-S_(3)motifs can serve as a highly efficient NORR ***1/MoS_(2)exhibits an NH_(3)yield rate of 337.5μmol·h^(−1)·cm^(−2)with a Faradaic efficiency of 90.6%at−0.6 V *** hydrogen electrode(RHE).Combined experiments and theoretical calculations reveal that Cu1-S3 motifs enable the effective activation and hydrogenation of NO through a mixed pathway and simultaneously retard proton coverage,contributing to the high activity and selectivity of Cu1/MoS_(2)for the NORR.

关键词： electrochemical NO reduction to NH_(3) Cu single-atom catalyst theoretical calculations