Coordination environments build up and tune a superior synergistic “genome” toward novel trifunctional (TM-N_(x)O_(4−x))@g- C_(16)N_(3)-H_(3): High-throughput inspection of ultra-high activity for water splitting and oxygen reduction reactions

Emerging as a prominent area of focus in energy conversion and storage technologies,the development of highly active metal-based single-atom catalysts(SACs)holds great significance in searching alternatives to replace precious metals toward the efficient,stable,and low-cost hydrogen evolution reaction(HER),as well as the oxygen evolution reaction(OER)and the oxygen reduction reaction(ORR).Combining the tremendous tunability of ligand and coordination environment with rich metal-based electrocatalysts can create breakthrough opportunities for achieving both high stability and activity.Herein,we propose a novel and stable holey graphene-like carbon nitride monolayer g-C_(16)N5(N_(4)@g-C_(16)N_(3))stoichiometries interestingly behaving as a natural substrate for constructing SACs((TM-N_(4))@g-C_(16)N_(3)),whose evenly distributed holes map rich and uniform nitrogen coordination positions with electron-rich lone pairs for anchoring transition metal(TM)atoms.Then,we employed density functional theory(DFT)calculations to systematically investigate the electrocatalytic activity of(TM-N_(4))@g-C_(16)N_(3) toward HER/OER/ORR,meanwhile considering the synergistic modulation of H-loading and O-coordination((TM-N_(x)O_(4-x))@g-C_(16)N_(3)^(-)H_(3),x=0–4).Together a“four-step procedure”screening mechanism with the first-principles high-throughput calculations,we find that(Rh-N_(4))and(Ir-N_(2)O_(2)-II)distributed on g-C_(16)N_(3)^(-)H_(3) can modulate the adsorption strength of the adsorbates,thus achieving the best HER/OER/ORR performance among 216 candidates,and the lowest overpotential of 0.098/0.3/0.46 V and 0.06/0.48/0.45 V,respectively.Additionally,the d-band center,crystal orbital Hamilton population(COHP),and molecular orbitals are used to reveal the OER/ORR activity source.Particularly,the Rh/Ir-d orbital is dramatically hybridized with the O-p orbital of the oxygenated adsorbates,so that the lone-electrons incipiently locate at the antibonding orbital pair up and populate the downward bonding orbital,allowing oxygenated intermediates to be adsorbed onto(TM-N_(x)O_(4-x))@g-C_(16)N_(3)^(-)H_(3) appropriately.

Joint load balancing and interference coordination in multi-antenna heterogeneous networks

In heterogeneous networks（Het Nets）, it is desirable to offload users from macro cells to small cells to achieve load balancing. However, the offloaded users suffer a strong inter-tier interference. To guarantee the performance of the offloaded users, the interference from macro cells should be carefully managed. In this paper, we jointly optimize load balancing and interference coordination in multi-antenna Het Nets. Different from previous works, instead of almost blank subframes（ABS） on which the macro cells waste time resource, the macro cells suppress the interference to the offloaded users by zero-forcing beamforming（ZFBF） on interference nulling subframes（INS）. Considering user association cannot be conduct frequently, we derive the long-term throughput of users over Rayleigh fading channels while previous works focused on instantaneous rate. From the perspective of the spectrum efficiency and user fairness, we formulate a long-term network-wide utility maximization problem. By decomposing the problem into two subproblems, we propose an efficient joint load balancing and interference coordination strategy. Simulation results show that our proposal can achieve good system performance gains over counterparts in term of the network utility, cell edge throughput and average throughput.

Mass transport in a thin layer of power-law fluid in an Eulerian coordinate system

The mass transport velocity in a thin layer of muddy fluid is studied theoretically. The mud motion is driven by a periodic pressure load on the free surface, and the mud is described by a power-law model. Based on the key assumptions of the shallowness and the small deformation, a perturbation analysis is conducted up to the second order to find the mean Eulerian velocity in an Eulerian coordinate system. The numerical iteration method is adopted to solve these non-linear equations of the leading order. From the numerical results, both the first-order flow fields and the second-order mass transport velocities are examined. The verifications are made by comparing the numerical results with experimental results in the literature, and a good agreement is confirmed.