General Synthesis of Composition-Tunable High-Entropy Amorphous Oxides Toward High Efficiency Oxygen Evolution Reaction.

High-entropy materials have attracted much attention in the electrocatalysis field due to their unique structure, high chemical activity, and compositional tunability. However, the harsh and complex synthetic methods limit the application of such materials. Herein, a universal non-equilibrium liquid-phase synthesis strategy is reported to prepare high-entropy amorphous oxide nanoparticles (HEAO-NPs), and the composition of HEAO-NPs can be precisely controlled from tri- to ten-component. The non-equilibrium synthesis environment provided by an excessively strong reducing agent overcomes the difference in the reduction potentials of various metal ions, resulting in the formation of HEAO-NPs with a nearly equimolar ratio. The oxygen evolution reaction (OER) performance of HEAO-NPs is further improved by adjusting the composition and optimizing the electronic structure. The Fe16Co32Ni32Mn10Cu10BOy exhibits a smaller overpotential (only 259 mV at 10 mA cm-2) and higher stability in OER compared with commercial RuO2. The amorphous high-entropy structure with an optimized concentration of iron makes the binding energy of CoNi shift to a higher direction, promotes the generation of high-valence active intermediates, and accelerates the OER kinetic process. The HEAO-NPs have promising application potential in the field of catalysis, biology, and energy storage, and this work provides a general synthesis method for composition-controllable high-entropy materials.

Advantages and Limitations of Monitoring Circulating Tumor DNA Levels to Predict the Prognosis of Patients Diagnosed With Gastric Cancer.

Next-generation sequencing-based genomic profiling facilitates biomarker detection by cell-free DNA (cfDNA) liquid biopsy. However, the efficiency of mutation calling and the prognostic value of cfDNA biomarkers are disputed. We investigated 24 patients with gastric cancer in this study, using a 605-gene sequencing panel to sequence their plasma cfDNA and tumor tissue DNA. The mutation concordance between plasma cfDNA and tumor tissue DNA was 70.6% in stage IV gastric cancer and 30.2% in stage III gastric cancer, indicating insufficient mutation detection rates in stage III and early-stage cancer. When compared with total cfDNA load and blood tumor mutation burden (bTMB), the variant allele frequencies (VAF) of commonly mutated genes are highly accurate in representing disease burden. Further, VAF are a better prognostic indicator compared with serum biomarkers including carcinoembryonic antigen (CEA), carbohydrate antigen 19-9 (CA19-9), cancer antigen 125 (CA125), and alpha-fetoprotein (AFP). The use of cfDNA in molecular profiling of patients allows prediction of patient survival and clinical response, as well as the development of personalized therapy regimens.

Amorphous High-entropy Non-precious metal oxides with surface reconstruction toward highly efficient and durable catalyst for oxygen evolution reaction.

High-entropy materials (HEMs) have attracted extensive interests in exploring multicomponent systems for highly efficient and durable catalysts. Tuning composition and configuration of HEMs provides untapped opportunities for accessing better catalytic performance. Herein, we report three amorphous high-entropy transition metal oxides catalysts with uniform composition through a simple and controllable liquid phase non-equilibrium reduction method. The self-made catalyst FeCoNiMnBOx exhibits excellent oxygen evolution performance, including a low overpotential (266 mV at 10 mA cm-2), small Tafel slope (64.5 mV dec-1) and extremely high stability (only 3.71% increase of potential after 100 h test and no current decay after cyclic voltammetry of 31,000 cycles). The outstanding performance can be attributed to the in-situ electrochemical activation induced surface reconstruction to form a stable oxyhydroxide surface layer, the cocktail effect (multi-metal synergy) brought by high entropy, and the advantages of amorphous structure itself. The outstanding catalytic properties of the new high-entropy amorphous metal oxide, as well as its advantages of low cost and simple preparation, suggest its great potential in water splitting.