Facile fabrication of heavily N-doped Zn0.67Cd0.33S nanocatalyst with congenital sulfur vacancies for efficient photocatalytic reduction of water and hexavalent chromium

IF 4.1 3区 化学 Q2 CHEMISTRY, PHYSICAL
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Abstract

Twinned zinc cadmium sulfide (ZnxCd1-xS) has been widely investigated for efficient Cr(VI) reduction and H2 production under light irradiation due to its inherent homojunctions. However, long-distance migration of charge carriers and relatively low conduction band level inevitably cause low photocatalytic reduction ability. Herein, we developed a DMF-involved one-step solvothermal strategy to introduce N heteroatoms into Zn0.67Cd0.33S crystals incorporated with dopant-induced S vacancies. The synergetic promotion of the elevated conduction band, coupled with the robust aggregation of interactants, effectively impeded the recombination behavior of charge carriers, leading to a notable increase in photocurrent density (∼2.4 times), electron density (∼2.8 times), and a higher photo-reducing potential. The optimal NZCS-10 demonstrated a superior photocatalytic Cr(VI) reduction efficiency of 99.32 % within 30 min, and rendered ca. 5.8- and 7.6-fold enhancement for H2 evolution rate under alkaline and acidic conditions, respectively. This study provided a universal strategy for gaining highly reductive transition metal sulfides with more active sites.

Abstract Image

轻松制备具有先天性硫空位的重氮掺杂 Zn0.67Cd0.33S 纳米催化剂,用于高效光催化还原水和六价铬
孪晶硫化镉锌(ZnxCd1-xS)因其固有的同质结而被广泛研究,用于在光照射下高效还原六价铬并产生 H2。然而,电荷载流子的长距离迁移和相对较低的导带电平不可避免地导致光催化还原能力低下。在此,我们开发了一种涉及 DMF 的一步溶热策略,将 N 杂原子引入到掺杂剂诱导 S 空位的 Zn0.67Cd0.33S 晶体中。协同作用促进了导带的升高,再加上相互作用物的强大聚合作用,有效地阻碍了电荷载流子的重组行为,从而显著提高了光电流密度(∼2.4 倍)、电子密度(∼2.8 倍)和更高的光电还原电位。最佳的 NZCS-10 在 30 分钟内的光催化还原六价铬效率高达 99.32%,在碱性和酸性条件下的 H2 演化率分别提高了约 5.8 倍和 7.6 倍。这项研究为获得具有更多活性位点的高还原性过渡金属硫化物提供了一种通用策略。
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来源期刊
CiteScore
7.90
自引率
7.00%
发文量
580
审稿时长
48 days
期刊介绍: JPPA publishes the results of fundamental studies on all aspects of chemical phenomena induced by interactions between light and molecules/matter of all kinds. All systems capable of being described at the molecular or integrated multimolecular level are appropriate for the journal. This includes all molecular chemical species as well as biomolecular, supramolecular, polymer and other macromolecular systems, as well as solid state photochemistry. In addition, the journal publishes studies of semiconductor and other photoactive organic and inorganic materials, photocatalysis (organic, inorganic, supramolecular and superconductor). The scope includes condensed and gas phase photochemistry, as well as synchrotron radiation chemistry. A broad range of processes and techniques in photochemistry are covered such as light induced energy, electron and proton transfer; nonlinear photochemical behavior; mechanistic investigation of photochemical reactions and identification of the products of photochemical reactions; quantum yield determinations and measurements of rate constants for primary and secondary photochemical processes; steady-state and time-resolved emission, ultrafast spectroscopic methods, single molecule spectroscopy, time resolved X-ray diffraction, luminescence microscopy, and scattering spectroscopy applied to photochemistry. Papers in emerging and applied areas such as luminescent sensors, electroluminescence, solar energy conversion, atmospheric photochemistry, environmental remediation, and related photocatalytic chemistry are also welcome.
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