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  1. Abstract Electrochemical oxygen reduction to hydrogen peroxide (H 2 O 2 ) in acidic media, especially in proton exchange membrane (PEM) electrode assembly reactors, suffers from low selectivity and the lack of low-cost catalysts. Here we present a cation-regulated interfacial engineering approach to promote the H 2 O 2 selectivity (over 80%) under industrial-relevant generation rates (over 400 mA cm −2 ) in strong acidic media using just carbon black catalyst and a small number of alkali metal cations, representing a 25-fold improvement compared to that without cation additives. Our density functional theory simulation suggests a “shielding effect” of alkali metal cations which squeeze away the catalyst/electrolyte interfacial protons and thus prevent further reduction of generated H 2 O 2 to water. A double-PEM solid electrolyte reactor was further developed to realize a continuous, selective (∼90%) and stable (over 500 hours) generation of H 2 O 2 via implementing this cation effect for practical applications.
    Free, publicly-accessible full text available December 1, 2023
  2. Abstract Electrochemical water oxidation reaction (WOR) to hydrogen peroxide (H 2 O 2 ) via a 2e − pathway provides a sustainable H 2 O 2 synthetic route, but is challenged by the traditional 4e − counterpart of oxygen evolution. Here we report a CO 2 /carbonate mediation approach to steering the WOR pathway from 4e − to 2e − . Using fluorine-doped tin oxide electrode in carbonate solutions, we achieved high H 2 O 2 selectivity of up to 87%, and delivered unprecedented H 2 O 2 partial currents of up to 1.3 A cm −2 , which represents orders of magnitude improvement compared to literature. Molecular dynamics simulations, coupled with electron paramagnetic resonance and isotope labeling experiments, suggested that carbonate mediates the WOR pathway to H 2 O 2 through the formation of carbonate radical and percarbonate intermediates. The high selectivity, industrial-relevant activity, and good durability open up practical opportunities for delocalized H 2 O 2 production.
    Free, publicly-accessible full text available December 1, 2023
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  4. Free, publicly-accessible full text available April 1, 2023
  5. Goaoc, Xavier ; Kerber, Michael (Ed.)
    We consider the following surveillance problem: Given a set P of n sites in a metric space and a set R of k robots with the same maximum speed, compute a patrol schedule of minimum latency for the robots. Here a patrol schedule specifies for each robot an infinite sequence of sites to visit (in the given order) and the latency L of a schedule is the maximum latency of any site, where the latency of a site s is the supremum of the lengths of the time intervals between consecutive visits to s. When k = 1 the problem is equivalent to the travelling salesman problem (TSP) and thus it is NP-hard. For k ≥ 2 (which is the version we are interested in) the problem becomes even more challenging; for example, it is not even clear if the decision version of the problem is decidable, in particular in the Euclidean case. We have two main results. We consider cyclic solutions in which the set of sites must be partitioned into 𝓁 groups, for some 𝓁 ≤ k, and each group is assigned a subset of the robots that move along the travelling salesman tour of the group atmore »equal distance from each other. Our first main result is that approximating the optimal latency of the class of cyclic solutions can be reduced to approximating the optimal travelling salesman tour on some input, with only a 1+ε factor loss in the approximation factor and an O((k/ε) ^k) factor loss in the runtime, for any ε > 0. Our second main result shows that an optimal cyclic solution is a 2(1-1/k)-approximation of the overall optimal solution. Note that for k = 2 this implies that an optimal cyclic solution is optimal overall. We conjecture that this is true for k ≥ 3 as well. The results have a number of consequences. For the Euclidean version of the problem, for instance, combining our results with known results on Euclidean TSP, yields a PTAS for approximating an optimal cyclic solution, and it yields a (2(1-1/k)+ε)-approximation of the optimal unrestricted (not necessarily cyclic) solution. If the conjecture mentioned above is true, then our algorithm is actually a PTAS for the general problem in the Euclidean setting. Similar results can be obtained by combining our results with other known TSP algorithms in non-Euclidean metrics.« less
    Free, publicly-accessible full text available January 1, 2023
  6. Abstract Oxygen reduction reaction towards hydrogen peroxide (H 2 O 2 ) provides a green alternative route for H 2 O 2 production, but it lacks efficient catalysts to achieve high selectivity and activity simultaneously under industrial-relevant production rates. Here we report a boron-doped carbon (B-C) catalyst which can overcome this activity-selectivity dilemma. Compared to the state-of-the-art oxidized carbon catalyst, B-C catalyst presents enhanced activity (saving more than 210 mV overpotential) under industrial-relevant currents (up to 300 mA cm −2 ) while maintaining high H 2 O 2 selectivity (85–90%). Density-functional theory calculations reveal that the boron dopant site is responsible for high H 2 O 2 activity and selectivity due to low thermodynamic and kinetic barriers. Employed in our porous solid electrolyte reactor, the B-C catalyst demonstrates a direct and continuous generation of pure H 2 O 2 solutions with high selectivity (up to 95%) and high H 2 O 2 partial currents (up to ~400 mA cm −2 ), illustrating the catalyst’s great potential for practical applications in the future.
    Free, publicly-accessible full text available December 1, 2022
  7. Electrochemical CO 2 or CO reduction to high-value C 2+ liquid fuels is desirable, but its practical application is challenged by impurities from cogenerated liquid products and solutes in liquid electrolytes, which necessitates cost- and energy-intensive downstream separation processes. By coupling rational designs in a Cu catalyst and porous solid electrolyte (PSE) reactor, here we demonstrate a direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction. With optimized edge-to-surface ratio, the Cu nanocube catalyst presents an unprecedented acetate performance in neutral pH with other liquid products greatly suppressed, delivering a maximal acetate Faradaic efficiency of 43%, partial current of 200 mA⋅cm −2 , ultrahigh relative purity of up to 98 wt%, and excellent stability of over 150 h continuous operation. Density functional theory simulations reveal the role of stepped sites along the cube edge in promoting the acetate pathway. Additionally, a PSE layer, other than a conventional liquid electrolyte, was designed to separate cathode and anode for efficient ion conductions, while not introducing any impurity ions into generated liquid fuels. Pure acetic acid solutions, with concentrations up to 2 wt% (0.33 M), can be continuously produced by employing the acetate-selective Cu catalyst in our PSE reactor.
  8. Free, publicly-accessible full text available December 1, 2022